Ultrafast control of light-matter interactions constitutes a crucial feature in view of new technological frontiers of information processing. However, conventional optical elements are either static or feature switching speeds that are extremely low with respect to the timescales at which it is possible to control light. Here, we exploit high-quality-factor engineered epsilon-near-zero (ENZ) modes of a metal-insulator-metal nanocavity to realize an all-optical ultrafast modulation of the reflectance of light at a tailored wavelength. Our approach is based on the presence of the two, spectrally separated, ENZ absorption resonances of the cavity. Optical pumping of the system at its high energy ENZ mode leads to a strong red-shift of the low energy mode because of the transient increase of the local dielectric function, which leads to a sub-3-ps control of the reflectance at a specific wavelength with a relative modulation depth approaching 120%.
Vibrational ultrastrong coupling (USC), where the light-matter coupling strength is comparable to the vibrational frequency of molecules, presents new opportunities to probe the interactions of molecules with zero-point fluctuations, harness cavity-enhanced chemical reactions, and develop novel devices in the mid-infrared regime. Here we use epsilon-near-zero nanocavities filled with a model polar medium (SiO$_2$) to demonstrate USC between phonons and gap plasmons. We present classical and quantum mechanical models to quantitatively describe the observed plasmon-phonon USC phenomena and demon…
Plasmon-mediated superradiance for molecules around metallic nanospheres was proposed ten years ago. However, its demonstration has not been achieved yet due to the experimental difficulty of positioning molecules, and the theoretical limitation to the enhanced collective rate of low excited molecules. In this Letter, we propose that the ultrafast plasmon-mediated superradiant pulses can be observed with strongly excited methylene blue molecules standing vertically inside gold nanoparticle-on-mirror nanocavities. Our simulations indicate that in this system the molecules could interact with ea…
The coupling between multiple nanocavities in close vicinity leads to hybridization of their modes. Stacked Metal/Insulator/Metal (MIM) nanocavities constitute a highly versatile and very interesting model system to study and engineer such mode coupling, since they can be realized by lithography-free fabrication methods with fine control on the optical and geometrical parameters. The resonant modes of such MIM cavities are epsilon-near-zero (ENZ) resonances, which are appealing for non-linear photophysics and a variety of applications. Here we study the hybridization of ENZ resonances in MIMIM…
Realizing remarkable tunability in optical properties without sacrificing speed is critical to obtain all optical ultrafast devices. In this work, we investigate the ultrafast temporal behavior of optically tunable epsilon-near-zero (ENZ) metamaterials, operating in the visible spectral range. To perform this the ultrafast dynamics of the hot electrons is acquired by femtosecond pump-probe spectroscopy and studied based on two-temperature model (2TM). We show that pumping with femtosecond pulses changes the effective permittivity of the metamaterial more than 400 %. This significant modulation…
Metal/Insulator/Metal nanocavities (MIMs) are highly versatile systems for nanometric light confinement and waveguiding, and their optical properties are mostly interpreted in terms of surface plasmon polaritons. Although classic electromagnetic theory accurately describes their behavior, it often lacks physical insight, letting some fundamental aspects of light interaction with these structures unexplored. In this work, we elaborate a quantum mechanical description of the MIM cavity as a double barrier quantum well. We identify the square of the imaginary part of the refractive index of the m…
Transparent conducting oxides have recently gained great attention as CMOS-compatible materials for applications in nanophotonics due to their low optical loss, metal-like behavior, versatile/tailorable optical properties, and established fabrication procedures. In particular, aluminum doped zinc oxide (AZO) is very attractive because its dielectric permittivity can be engineered over a broad range in the near infrared and infrared. However, despite all these beneficial features, the slow (> 100 ps) electron-hole recombination time typical of these compounds still represents a fundamental limi…
Epsilon-near-zero (ENZ) materials have shown significant potential for nonlinear optical applications due to their ultrafast hot carriers and consequent optical nonlinearity enhancement. Modified poly(3,4-ethylenedioxythiophene) (PEDOT) films show metallic characteristics and a resultant ENZ wavelength near 1550nm through polar solvent treatment and annealing. The metallic PEDOT film exhibits an intrinsic optical nonlinear response that is comparable to gold and 100-fold higher than typical inorganic semiconductor ENZ materials due to π-conjugated delocalized electrons. Hot carriers generate a…
New propagation regimes for light arise from the ability to tune the dielectric permittivity to extremely low values. Here we demonstrate a universal approach based on the low linear permittivity values attained in the epsilon-near-zero (ENZ) regime for enhancing the nonlinear refractive index, which enables remarkable light-induced changes of the material properties. Experiments performed on Al-doped ZnO (AZO) thin films show a six-fold increase of the Kerr nonlinear refractive index ($n_2$) at the ENZ wavelength, located in the 1300 nm region. This in turn leads to ultrafast light-induced re…
The ultrafast changes of material properties induced by short laser pulses can lead to frequency shift of reflected and transmitted radiation. Recent reports highlight how such a frequency shift is enhanced in the spectral regions where the material features a near-zero real part of the permittivity. Here we investigate the frequency shift for fields generated by four-wave mixing with a nonlinear polarisation oscillating at twice the pump frequency. In our experiment we observe a frequency shift of more than 60 nm (compared to the pulse width of ~40 nm) for the phase conjugated radiation gener…
Engineered core-shell cylinders are good candidates for applications in invisibility and cloaking.In particular, hyperbolic nanotubes demonstrate tunable ultra-low scattering cross section in the visible spectral range. In this work we investigate the limits of validity of the condition for invisibility, which was shown to rely on reaching an epsilon near zero in one of the components of the effective permittivity tensor of the anisotropic metamaterial cavity. For incident light polarized perpendicularly to the scatterer axis, critical deviations are found in low-birefringent arrangements and …
We propose a scheme to realize nonlinear coherent perfect absorption (CPA) at the nanoscale using epsilon-near-zero (ENZ) plasmonic waveguides. The general conditions to achieve CPA in a linear ENZ plasmonic waveguide are analyzed and presented. The proposed ENZ waveguides support an effective ENZ response at their cut-off frequency, where the CPA effect occurs under the illumination of two counter-propagating plane waves with equal amplitudes and appropriate phase distributions. In addition, the strong and uniform field enhancement inside the nanochannels of the waveguides at the ENZ resonanc…
We propose tunable nonlinear antennas based on an epsilon-near-zero material with a large optical nonlinearity. We show that the absorption and scattering cross sections of the antennas can be controlled dynamically from a nearly superscatterer to a nearly superabsorber by changing the intensity of the laser beam. Moreover, we demonstrate that a hybrid nonlinear antenna, composed of epsilon-near-zero and high-index dielectric materials, exhibits nonreciprocal radiation patterns because of broken spatial inversion symmetry and large optical nonlinearity of the epsilon-near-zero material. By cha…
For decades, nonlinear optics has been used to control the frequency and propagation of light in unique ways enabling a wide range of applications such as ultrafast lasing, sub-wavelength imaging, and novel sensing methods. Through this, a key thread of research in the field has always been the development of new and improved nonlinear materials to empower these applications. Recently, epsilon-near-zero (ENZ) materials have emerged as a potential platform to enhanced nonlinear interactions, bolstered in large part due to the extreme refractive index tuning (Δn~ 0.1 - 1) of sub-micron thick fil…
Dynamical materials that capable of responding to optical stimuli have always been pursued for designing novel photonic devices and functionalities, of which the response speed and amplitude as well as integration adaptability and energy effectiveness are especially critical. Here we show ultrafast pulse generation by exploiting the ultrafast and sensitive nonlinear dynamical processes in tunably solution-processed colloidal epsilon-near-zero (ENZ) transparent conducting oxide (TCO) nanocrystals (NCs), of which the potential respond response speed is >2 THz and modulation depth is ~23% pumped …
An optical topological transition is defined as the change in the photonic isofrequency surface around epsilon-near-zero (ENZ) frequencies which can considerably change the spontaneous emission of a quantum emitter placed near a metamaterial slab. Here, we show that due to the strong Kerr nonlinearity at ENZ frequencies, a high power pulse can induce a sudden transition in the topology of the iso-frequency dispersion curve, leading to a significant change in the transmission of propagating as well as evanescent waves through the metamaterial slab. This evanescent wave switch effect allows for …
Epsilon-near-zero (ENZ) materials have emerged as viable platforms for strong nonlinear optical (NLO) interactions. The NLO phase shift in materials exhibiting an ENZ condition is extremely large, however, direct experimental measurements of the magnitude and time dynamics of this phenomenon, particularly nondegenerate NLO phase shifts, have so far been lacking. Here, we directly measure the NLO phase shift of an Indium-Tin-Oxide (ITO) thin film using three different techniques. By characterizing the excitation-induced, time resolved Beam Deflection (BD) of a probe beam, we measure the nondege…
Nonreciprocal ENZ-Dielectric Bilayers: Enhancement of Nonreciprocity from a Nonlinear Transparent Conducting Oxide Thin Film at Epsilon-Near-Zero (ENZ) Frequency
Nanophotonics and metamaterials have revolutionised the way we think about optical space (epsilon, mu), enabling us to engineer the refractive index almost at will, to confine light to the smallest of the volumes, and to manipulate optical signals with extremely small footprints and energy requirements. Significant efforts are now devoted to finding suitable materials and strategies for the dynamic control of the optical properties. Transparent conductive oxides exhibit large ultrafast nonlinearities under both interband and intraband excitations. Here, we show that combining these two effects…
Femtosecond all-optical polarization manipulation of harmonic generation in an anisotropic strongly coupled plasmon-epsilon-near-zero metasurface
Key Laboratory for Physical Electronics and Devices of the Ministry of Education and Shaanxi Key Lab of Information Photonic Technique, School of Electronic Science and Engineering, Xi’an Jiaotong University（教育部光电技术与器件重点实验室、陕西省信息光子技术重点实验室，西安交通大学电子科学与工程学院）
Transparent conductive oxides such as indium tin oxide (ITO) bear the potential to deliver efficient all-optical functionality due to their record-breaking optical nonlinearity at epsilon near zero (ENZ) wavelengths. All-optical applications generally involve more than one beam, but the coherent interaction between beams has not previously been discussed in materials with a hot electron nonlinearity. Here we study the optical nonlinearity at ENZ in ITO and show that spatial and temporal interference has important consequences in a two beam geometry. Our pump-probe results reveal a polarization…
Thermo-optic dynamics of effective epsilon-near-zero media
École Polytechnique Fédérale de Lausanne (EPFL)（洛桑联邦理工学院）；City University of Hong Kong (Dongguan)（香港城市大学（东莞））；Sun Yat-sen University（中山大学）；Università di Pavia（帕维亚大学）
Novel materials, with enhanced light-matter interaction capabilities, play an essential role in achieving the lofty goals of nonlinear optics. Recently, Epsilon-Near-Zero (ENZ) media have emerged as a promising candidate to enable the enhancement of several nonlinear processes including refractive index modulation and harmonic generation. Here, we analyze the optical nonlinearity of ENZ media to clarify the commonalities with other nonlinear media and its unique properties. We focus on transparent conducting oxides (TCOs) as the family of ENZ media with near zero permittivity in the near-infra…
All optical switches offer advanced control over the properties of light at ultrafast timescales using optical pulses as both the signal and the control. Limited only by material response times, these switches can operate at terahertz speeds, essential for technology-driven applications such as all-optical signal processing and ultrafast imaging, as well as for fundamental studies such as frequency translation and novel optical media concepts such as photonic time crystals. In conventional systems, the switching time is determined by the relaxation response of a single active material, which i…
