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Boltasseva, Alexandra

Publications and source records attributed to Boltasseva, Alexandra.

At least 37 records · Page 2

Near-zero-index ultra-fast pulse characterization

Transparent conducting oxides exhibit giant optical nonlinearities in the near-infrared window where their linear index approaches zero. Despite the magnitude and speed of these nonlinearities, a “killer” optical application for these compounds has yet to be found. Because of the absorptive nature of the typically used intraband transitions, out-of-plane configurations with short optical paths should be considered. In this direction, we propose an alternative frequency-resolved optical gating scheme for the characterization of ultra-fast optical pulses that exploits near-zero-index aluminium zinc oxide thin films. Besides the technological advantages in terms of manufacturability and cost, our system outperforms commercial modules in key metrics, such as operational bandwidth, sensitivity, and robustness. The performance enhancement comes with the additional benefit of simultaneous self-phase-matched second and third harmonic generation. Because of the fundamental importance of novel methodologies to characterise ultra-fast events, our solution could be of fundamental use for numerous research labs and industries.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Zinc oxide (ZnO) hybrid metasurfaces exhibiting broadly tunable topological properties

Extreme light confinement observed in periodic photonic structures, such as the vortex singularities in momentum (k) space, has been associated with their topological nature. Consequently, by exploiting and tuning their topological properties, optical metasurfaces have been demonstrated as an attractive platform for active photonics. However, given the fact that most active media under external excitations can only provide limited refractive index change, the potential advancements offered by the topological character of active metasurfaces have remained mostly unexplored. Zinc oxide (ZnO), which has recently exhibited optically-induced extraordinarily large permittivity modulations at visible and near-infrared frequencies, is an excellent active material for dynamic metasurfaces exhibiting strong tuning. This work demonstrates that a hybrid metasurface consisting of an array of ZnO nanodisks on a silver backplane displays broadly tunable topological properties. In particular, by performing k-space scattering simulations using measured pump-fluence-dependent material properties of ZnO, we study in detail the light reflection from the hybrid metasurface. Our results validate that the large k-space topology tuning of the metasurface can result in enormously strong polarization manipulation of near-infrared light in the vicinity of the topological features. The observed polarization switching effect is highly sensitive to the polarization and wavelength of an incident wave, owing to the symmetry and dispersion characteristics of the proposed system. Our study indicates that leveraging a combination of the extraordinary material properties and the k-space topology, hybrid metasurfaces based on ZnO may open new avenues for creating all-optical switchable metadevices.

36 MATERIALS SCIENCE↗

Room-temperature single-photon emitters in silicon nitride

Single-photon emitters are essential in enabling several emerging applications in quantum information technology, quantum sensing, and quantum communication. Scalable photonic platforms capable of hosting intrinsic or embedded sources of single-photon emission are of particular interest for the realization of integrated quantum photonic circuits. Here, we report on the observation of room-temperature single-photon emitters in silicon nitride (SiN) films grown on silicon dioxide substrates. Photophysical analysis reveals bright (>10 5 counts/s), stable, linearly polarized, and pure quantum emitters in SiN films with a second-order autocorrelation function value at zero time delay g (2) (0) below 0.2 at room temperature. We suggest that the emission originates from a specific defect center in SiN because of the narrow wavelength distribution of the observed luminescence peak. Single-photon emitters in SiN have the potential to enable direct, scalable, and low-loss integration of quantum light sources with a well-established photonic on-chip platform.

42 ENGINEERING↗

Machine learning framework for quantum sampling of highly constrained, continuous optimization problems

In recent years, there is growing interest in using quantum computers for solving combinatorial optimization problems. In this work, we developed a generic, machine learning-based framework for mapping continuous-space inverse design problems into surrogate quadratic unconstrained binary optimization (QUBO) problems by employing a binary variational autoencoder and a factorization machine. The factorization machine is trained as a low-dimensional, binary surrogate model for the continuous design space and sampled using various QUBO samplers. Using the D-Wave Advantage hybrid sampler and simulated annealing, we demonstrate that by repeated resampling and retraining of the factorization machine, our framework finds designs that exhibit figures of merit exceeding those of its training set. We showcase the framework’s performance on two inverse design problems by optimizing (i) thermal emitter topologies for thermophotovoltaic applications and (ii) diffractive meta-gratings for highly efficient beam steering. This technique can be further scaled to leverage future developments in quantum optimization to solve advanced inverse design problems for science and engineering applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Extraordinarily large permittivity modulation in zinc oxide for dynamic nanophotonics

The dielectric permittivity of a material encapsulates the essential physics of light-matter interaction into the material's local response to optical excitation. Photo-induced modulation of the permittivity can enable an unprecedented level of control over the phase, amplitude, and polarization of light. Therefore, the detailed dynamic characterization of technology-relevant materials with substantially tunable optical properties and fast response times is a crucial step to realize tunable optical devices. This work reports on the extraordinarily large permittivity changes in zinc oxide thin films (up to similar to 3.6 relative change in the real part of the dielectric permittivity at 1600 nm wavelength) induced by optically generated free carriers. We demonstrate broadband reflectance modulation up to 70% in metal-backed oxide mirrors at the telecommunication wavelengths, with picosecond-scale relaxation times. The epsilon near zero points of the films can be dynamically shifted from 8.5 mm to 1.6 mm by controlling the pump fluence. Additionally, the modulation can be selectively enhanced at specific wavelengths employing metal-backed zinc oxide disks while maintaining picosecond-scale switching times. This work provides insights into the free-carrier assisted permittivity modulation in zinc oxide and could enable the realization of novel dynamic devices for beam-steering, polarizers, and spatial light modulators.

36 MATERIALS SCIENCE↗

Dynamically controlled random lasing with colloidal titanium carbide MXene

Control of lasing properties through tailorable and dynamically tunable materials and reconfigurable compositions can augment the performance of random lasers for a wide range of applications. Here, a colloid of randomly dispersed weakly scattering single-layer titanium carbide (Ti 3 C 2 T x ) MXene flakes embedded within rhodamine 101 gain medium is experimentally shown to provide feedback for random lasing. Additionally, in contrast to previously reported random laser systems where the optical properties of scatterers are static, the relative permittivity of Ti 3 C 2 T x MXene flakes can be varied under optical pumping due to the saturable absorption properties. Numerical simulations indicate that the observed nonlinear response of Ti 3 C 2 T x MXene flakes enables dynamically tunable random lasing. Thus, pumping the Ti 3 C 2 T x MXene flakes with a second optical source decreases the gain threshold required to obtain random lasing. Also, using numerical simulations, it is shown that the control over the intensity of the second pump enables tuning the field distribution of the random lasing modes. Considering the diversity of the MXenes family, the proposed MXene colloidal metamaterial design opens up a new avenue to advanced control of lasing properties for photonic applications.

36 MATERIALS SCIENCE↗

On-Chip Single-Layer Integration of Diamond Spins with Microwave and Plasmonic Channels

On-chip scalable integration represents a major challenge for practical quantum devices. One particular challenge is to implement on-chip optical readout of spins in diamond. This readout requires simultaneous application of optical and microwave fields along with the efficient collection of fluorescence. These requirements are typically met using bulk optical components and dedicated microwave lines. Here, we experimentally demonstrate an on-chip integrated interface for diamond nitrogen vacancy (NV) spin-state preparation and readout, implemented in a planar single layer with only one patterning step. A nanodiamond with NV centers is positioned inside a v-groove waveguide milled in a thick gold film. The gold film carries the microwave control signal, while the v-groove acts as a fluorescence collector and, potentially, as an integrated pump filter. Hence, the device dimensions and fabrication complexity are substantially reduced. Our approach fosters further development of ultracompact nanoscale quantum sensors and quantum information processing devices on a monolithic platform.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Broadband Ultrafast Dynamics of Refractory Metals: TiN and ZrN

Transition metal nitrides have recently gained attention in the fields of plasmonics, plasmon-enhanced photocatalysis, photothermal applications, and nonlinear optics because of their suitable optical properties, refractory nature, and large laser damage thresholds. Here we report comparative studies of the transient response of films of titanium nitride (TiN), zirconium nitride (ZrN), and gold (Au) under femtosecond excitation. Broadband transient optical characterization helps to adjudicate earlier, somewhat inconsistent reports regarding hot electron lifetimes based upon single wavelength measurements. These pump–probe experiments show sub-picosecond transient dynamics only within the epsilon-near-zero window of the refractory metals. The dynamics are dominated by photoinduced interband transitions resulting from ultrafast electron energy redistribution. The enhanced reflection modulation in the epsilon-near-zero window makes it possible to observe the ultrafast optical response of these films at low pump fluences. These results indicate that electron–phonon coupling in TiN and ZrN is 25–100 times greater than in Au. Strong electron–phonon coupling drives the sub-picosecond optical response and facilitates greater lattice heating compared to Au, making TiN and ZrN promising for photothermal applications. The spectral response and dynamics of TiN and ZrN are only weakly sensitive to pump fluence and pump excitation energy. However, the magnitude of the response is much greater at higher pump photon energies and higher fluences, reaching peak observed values of 15% in TiN and 50% in ZrN in the epsilon-near-zero window.

36 MATERIALS SCIENCE↗

Determining plasmonic hot-carrier energy distributions via single-molecule transport measurements

Hot carriers in plasmonic nanostructures, generated via plasmon decay, play key roles in applications such as photocatalysis and in photodetectors that circumvent bandgap limitations. However, direct experimental quantification of steady-state energy distributions of hot carriers in nanostructures has so far been lacking. We present transport measurements from single-molecule junctions, created by trapping suitably chosen single molecules between an ultrathin gold film supporting surface plasmon polaritons and a scanning probe tip, that can provide quantification of plasmonic hot-carrier distributions. Our results show that Landau damping is the dominant physical mechanism of hot-carrier generation in nanoscale systems with strong confinement. The technique developed in this work will enable quantification of plasmonic hot-carrier distributions in nanophotonic and plasmonic devices.

Science & Technology - Other Topics↗

Ultrafast quantum photonics enabled by coupling plasmonic nanocavities to strongly radiative antennas

Quantum emitters coupled to plasmonic nanostructures can act as exceptionally bright sources of single photons, operating at room temperature. Plasmonic mode volumes supported by these nanostructures can be several orders of magnitude smaller than the cubic wavelength, which leads to dramatically enhanced light–matter interactions and drastically increased photon production rates. However, when increasing the light localization further, these deeply subwavelength modes may in turn hinder the fast outcoupling of photons into free space. Plasmonic hybrid nanostructures combining a highly confined cavity mode and a larger antenna mode circumvent this issue. We establish the fundamental limits for quantum emission enhancement in such systems and find that the best performance is achieved when the cavity and antenna modes differ significantly in size. We experimentally support this idea by photomodifying a nanopatch antenna deterministically assembled around a nanodiamond known to contain a single nitrogen–vacancy (NV) center. As a result, the cavity mode shrinks, further shortening the NV fluorescence lifetime and increasing the single-photon brightness. Our analytical and numerical simulation results provide intuitive insight into the operation of these emitter–cavity–antenna systems and show that this approach could lead to single-photon sources with emission rates up to hundreds of THz and efficiencies close to unity.

47 OTHER INSTRUMENTATION↗

Adiabatic frequency shifting in epsilon-near-zero materials: the role of group velocity

The conversion of a photon’s frequency has long been a key application area of nonlinear optics. It has been discussed how a slow temporal variation of a material’s refractive index can lead to the adiabatic frequency shift (AFS) of a pulse spectrum. Such a rigid spectral change has relevant technological implications, for example, in ultrafast signal processing. Here, we investigate the AFS process in epsilon-near-zero (ENZ) materials and show that the frequency shift can be achieved in a shorter length if operating in the vicinity of R e { ε <#comment/> r } = 0 . We also predict that, if the refractive index is induced by an intense optical pulse, the frequency shift is more efficient for a pump at the ENZ wavelength. Remarkably, we show that these effects are a consequence of the slow propagation speed of pulses at the ENZ wavelength. Our theoretical predictions are validated by experiments obtained for the AFS of optical pulses incident upon aluminum zinc oxide thin films at ENZ. Our results indicate that transparent metal oxides operating near the ENZ point are good candidates for future frequency conversion schemes.

36 MATERIALS SCIENCE↗