Low-loss and high-index contrast ultraviolet-C free-standing waveguides made of thermal silicon oxide.

Photonics in the ultraviolet provides an avenue for key advances in biosensing, pharmaceutical research, and environmental sensing. However, despite recent progress in photonic integration, a technological solution to fabricate photonic integrated circuits (PICs) operating in the UV-C wavelength range, namely, between 200 and 280 nm, remains elusive. Filling this gap will open opportunities for new applications, particularly in healthcare. A major challenge has been to identify materials with low optical absorption loss in this wavelength range that are at the same time compatible with waveguide design and large-scale fabrication. In this work, we unveil that thermal silicon oxide (TOX) on a silicon substrate is a potential candidate for integrated photonics in the UV-C, by removing the silicon substrate under selected regions to form single-side suspended ridge waveguides. We provide design guidelines for low-loss waveguide geometries, avoiding wrinkling due to residual intrinsic stress, and experimentally demonstrate waveguides that exhibit optical propagation losses below 3 and 4 dB/cm at a wavelength of 266 nm with claddings of air and water, respectively. This result paves the way for on-chip UV-C biological sensing and imaging.

Mode-Specific Coupling of Nanoparticle-on-Mirror Cavities with Cylindrical Vector Beams.

Nanocavities formed by ultrathin metallic gaps permit the reproducible engineering and enhancement of light-matter interaction, with mode volumes reaching the smallest values allowed by quantum mechanics. While the enhanced vacuum field in metallic nanogaps has been firmly evidenced, fewer experimental reports have examined the far-field to near-field input coupling under strongly focused laser beam. Here, we experimentally demonstrate selective excitation of nanocavity modes controlled by the polarization and frequency of the laser beam. We reveal mode selectivity by recording confocal maps of Raman scattering excited by cylindrical vector beams, which are compared to the known excitation near-field patterns. Our measurements reveal the transverse vs longitudinal polarization of the excited antenna mode and how the input coupling rate depends on laser wavelength. The method introduced here is easily applicable to other experimental scenarios, and our results help connect far-field with near-field parameters in quantitative models of nanocavity-enhanced phenomena.

Molecular Vibration Explorer: an Online Database and Toolbox for Surface-Enhanced Frequency Conversion and Infrared and Raman Spectroscopy.

We present Molecular Vibration Explorer, a freely accessible online database and interactive tool for exploring vibrational spectra and tensorial light-vibration coupling strengths of a large collection of thiolated molecules. The "Gold" version of the database gathers the results from density functional theory calculations on 2800 commercially available thiol compounds linked to a gold atom, with the main motivation to screen the best molecules for THz and mid-infrared to visible upconversion. Additionally, the "Thiol" version of the database contains results for 1900 unbound thiolated compounds. They both provide access to a comprehensive set of computed spectroscopic parameters for all vibrational modes of all molecules in the database. The user can simultaneously investigate infrared absorption, Raman scattering, and vibrational sum- and difference-frequency generation cross sections. Molecules can be screened for various parameters in custom frequency ranges, such as a large Raman cross-section under a specific molecular orientation, or a large orientation-averaged sum-frequency generation (SFG) efficiency. The user can select polarization vectors for the electromagnetic fields, set the orientation of the molecule, and customize parameters for plotting the corresponding IR, Raman, and sum-frequency spectra. We illustrate the capabilities of this tool with selected applications in the field of surface-enhanced spectroscopy.

Nonlinear characterization of a silicon integrated Bragg waveguide filter.

Bragg waveguides are promising optical filters for pump suppression in spontaneous four-wave mixing (FWM) photon sources. In this work, we investigate the generation of unwanted photon pairs in the filter itself. We do this by taking advantage of the relation between spontaneous and classical FWM, which allows for the precise characterization of the nonlinear response of the device. The pair generation rate estimated from the classical measurement is compared with the theoretical value calculated by means of a full quantum model of the filter, which also allows investigation of the spectral properties of the generated pairs. We find a good agreement between theory and experiment, confirming that stimulated FWM is a valuable approach to characterize the nonlinear response of an integrated filter, and that the pairs generated in a Bragg waveguide are not a serious issue for the operation of a fully integrated nonclassical source.

Two-Color Pump-Probe Measurement of Photonic Quantum Correlations Mediated by a Single Phonon.

We propose and demonstrate a versatile technique to measure the lifetime of the one-phonon Fock state using two-color pump-probe Raman scattering and spectrally resolved, time-correlated photon counting. Following pulsed laser excitation, the n=1 phonon Fock state is probabilistically prepared by projective measurement of a single Stokes photon. The detection of an anti-Stokes photon generated by a second, time-delayed laser pulse probes the phonon population with subpicosecond time resolution. We observe strongly nonclassical Stokes-anti-Stokes correlations, whose decay maps the single phonon dynamics. Our scheme can be applied to any Raman-active vibrational mode. It can be modified to measure the lifetime of n≥1 Fock states or the phonon quantum coherences through the preparation and detection of two-mode entangled vibrational states.

Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots.

Photoluminescence blinking--random switching between states of high (ON) and low (OFF) emissivities--is a universal property of molecular emitters found in dyes, polymers, biological molecules and artificial nanostructures such as nanocrystal quantum dots, carbon nanotubes and nanowires. For the past 15 years, colloidal nanocrystals have been used as a model system to study this phenomenon. The occurrence of OFF periods in nanocrystal emission has been commonly attributed to the presence of an additional charge, which leads to photoluminescence quenching by non-radiative recombination (the Auger mechanism). However, this 'charging' model was recently challenged in several reports. Here we report time-resolved photoluminescence studies of individual nanocrystal quantum dots performed while electrochemically controlling the degree of their charging, with the goal of clarifying the role of charging in blinking. We find that two distinct types of blinking are possible: conventional (A-type) blinking due to charging and discharging of the nanocrystal core, in which lower photoluminescence intensities correlate with shorter photoluminescence lifetimes; and a second sort (B-type), in which large changes in the emission intensity are not accompanied by significant changes in emission dynamics. We attribute B-type blinking to charge fluctuations in the electron-accepting surface sites. When unoccupied, these sites intercept 'hot' electrons before they relax into emitting core states. Both blinking mechanisms can be electrochemically controlled and completely suppressed by application of an appropriate potential.

Dual-color electroluminescence from dot-in-bulk nanocrystals.

The emission color from colloidal semiconductor nanocrystals (NCs) is usually tuned through control of particle size, while multicolor emission is obtained by mixing NCs of different sizes within an emissive layer. Here, we demonstrate that recently introduced "dot-in-bulk" (DiB) nanocrystals can emit two-color light under both optical excitation and electrical injection. We show that the effective emission color can be controlled by adjusting the relative amplitudes of the core and shell emission bands via the intensity of optical excitation or applied bias in the cases of photoluminescence (PL) and electroluminescence (EL), respectively. To investigate the role of nonradiative carrier losses due to trapping at intragap states, we incorporate DiB NCs into functional light-emitting diodes and study their PL as a function of applied bias below the EL excitation threshold. We show that voltage-dependent changes in core and shell emissions are not due to the applied electric field but rather arise from the transfer of charges between the anode and the NC intragap trap sites. The changes in the occupancy of trap states can be described in terms of the raising (lowering) of the Fermi level for reverse (direct) bias. We find that the applied voltage affects the overall PL intensity primarily via the electron-trapping channel while bias-induced changes in hole-trapping play a less significant role, limited to a weak effect on core emission.

Electrochemical control of two-color emission from colloidal dot-in-bulk nanocrystals.

Colloidal "dot-in-bulk" nanocrystals (DiB NCs) consist of a quantum confined core embedded into a bulklike shell of a larger energy gap. The first reported example of this class of nanostructures are CdSe/CdS DiB NCs that are capable of producing tunable two-color emission under both weak continuous-wave optical excitation and electrical charge injection. This property is a consequence of a Coulomb blockade mechanism, which slows down dramatically intraband relaxation of shell-localized holes when the core is already occupied by a hole. Here, we demonstrate electrochemical control of dual emission from DiB NCs. Spectro-electrochemical (SEC) experiments are used to tune and probe the photoluminescence (PL) intensity and branching between the core and the shell emission channels as a function of applied electrochemical potential (VEC). To interpret the SEC data we develop a model that describes the changes in the intensities of the shell and core PL bands by relating them to the occupancies of electron and hole traps. Specifically, application of negative electrochemical potentials under which the Fermi level is shifted upward in energy leads to passivation of electron traps at the surface of the CdS shell thereby increasing the total PL quantum yield by favoring the shell emission. Simultaneously, the emission color changes from red (VEC = 0) through yellow to green (VEC = -1). Time-resolved PL measurements indicate that as the Fermi level approaches the NC conduction band-edge electrons are injected into the NC quantized states, which leads to typical signatures of negative trions observed under optical excitation. Application of positive potentials leads to activation of electron traps, which quenches both core and shell PL and leads to the reduction of the overall PL quantum efficiency. A high sensitivity of emission intensity (especially pronounced for the shell band) and the apparent emission color of DiB NCs to local electrochemical environment can enable interesting applications of these novel nanostructures in areas of imaging and sensing including, for example, ratiometric probing of intracellular pH.

Efficient, compact and low loss thermo-optic phase shifter in silicon.

We design a resistive heater optimized for efficient and low-loss optical phase modulation in a silicon-on-insulator (SOI) waveguide and characterize the fabricated devices. Modulation is achieved by flowing current perpendicular to a new ridge waveguide geometry. The resistance profile is engineered using different dopant concentrations to obtain localized heat generation and maximize the overlap between the optical mode and the high temperature regions of the structure, while simultaneously minimizing optical loss due to free-carrier absorption. A 61.6 µm long phase shifter was fabricated in a CMOS process with oxide cladding and two metal layers. The device features a phase-shifting efficiency of 24.77 ± 0.43 mW/π and a -3 dB modulation bandwidth of 130.0 ± 5.59 kHz; the insertion loss measured for 21 devices across an 8-inch wafer was only 0.23 ± 0.13 dB. Considering the prospect of densely integrated photonic circuits, we also quantify the separation necessary to isolate thermo-optic devices in the standard 220 nm SOI platform.

Experimental demonstration of broadband Lorentz non-reciprocity in an integrable photonic architecture based on Mach-Zehnder modulators.

Lorentz reciprocity is a direct consequence of Maxwell equations governing the propagation of light in passive linear media with symmetric permittivity and permeability tensors. Here, we demonstrate the first active optical isolator and circulator implemented in a linear and reciprocal material platform using commercial Mach-Zehnder modulators. In a proof-of-principle experiment based on single-mode polarization-maintaining fibers, we achieve more than 12.5 dB isolation over an unprecedented 8.7 THz bandwidth at telecommunication wavelengths, with only 9.1 dB total insertion loss. Our architecture provides a practical answer to the challenge of non-reciprocal light routing in photonic integrated circuits.

Heralded single-phonon preparation, storage, and readout in cavity optomechanics.

We show how to use the radiation pressure optomechanical coupling between a mechanical oscillator and an optical cavity field to generate in a heralded way a single quantum of mechanical motion (a Fock state). Starting with the oscillator close to its ground state, a laser pumping the upper motional sideband produces correlated photon-phonon pairs via optomechanical parametric down-conversion. Subsequent detection of a single scattered Stokes photon projects the macroscopic oscillator into a single-phonon Fock state. The nonclassical nature of this mechanical state can be demonstrated by applying a readout laser on the lower sideband to map the phononic state to a photonic mode and performing an autocorrelation measurement. Our approach proves the relevance of cavity optomechanics as an enabling quantum technology.

Dynamic hole blockade yields two-color quantum and classical light from dot-in-bulk nanocrystals.

Semiconductor nanocrystals (NCs) are an emerging class of color-tunable, solution-processable, room-temperature single-photon sources. Photon antibunching in NCs arises from suppression of multiphoton emission by nonradiative Auger recombination. Here, we demonstrate a new antibunching mechanism-dynamic Coulomb blockade-which allows for generating both quantum and classical light from the same NC without detrimental effects of Auger decay. This mechanism is realized in novel dot-in-bulk (DiB) nanostructures comprising a quantum-confined CdSe core overcoated with a thick, bulk-like CdS shell. The presence of one hole in the core suppresses the capture of the second hole forcing it to recombine in the shell region. Under weak excitation, these NCs emit red antibunched light (core emission). At higher pump levels they exhibit an additional green band (shell emission) with bulk-like, Poissonian photon statistics. The unusual versatility of these novel nanoscale light sources, that combine mutually correlated channels for quantum and classical emission and additionally allow for facile tunability of effective color, opens new interesting opportunities for a range of applications from quantum optics to sensing and nanoscale imaging.

Integrated coplanar waveguide coil on diamond for enhanced homogeneous broadband NV magnetometry.

Nitrogen-vacancy (NV) centers in diamond have emerged as promising quantum sensors due to their highly coherent and optically addressable spin states with potential applications in high-sensitivity magnetometry. Homogeneously addressing large ensembles of NV centers offers clear benefit in terms of sensing precision as well as in fundamental studies of collective effects. Such experiments require a spatially uniform, intense, and broadband microwave field that can be difficult to generate. Previous approaches, such as copper wires, loop coils, and planar structures, have shown limitations in field homogeneity, bandwidth, and integration in compact devices. In this paper, we present a coplanar waveguide (CPW) gold coil patterned on a 3 × 3 mm 2 diamond substrate, offering full integration, enhanced stability, and broad bandwidth suitable for various NV sensing applications. Coil fabricated on diamond offers several advantages for magnetometry with NV centers ensemble, including enhanced heat dissipation, seamless integration, scalability, and miniaturization potential. We optimize critical geometrical parameters to achieve a homogeneous magnetic field with a coefficient of variation of less than 6% over an area of 0.5 mm 2 and present experimental results confirming the performance of the proposed CPW coil.

In recent years, there has been significant interest in using nitrogen-vacancy (NV) centers in diamond as quantum sensors for high-sensitivity magnetometry. These NV centers, particularly the negatively charged ones, offer promising applications due to their coherent spin states that can be manipulated using microwave fields and optically detected magnetic resonance techniques. However, to improve measurement precision and signal-to-noise ratio, it's advantageous to address large ensembles of NV centers, which requires a spatially uniform, intense, and broadband microwave field. Various methods, such as copper wires, loop coils, and planar structures, have been explored to achieve this, but with limited capability. To address their limitations, a coplanar waveguide (CPW) gold coil patterned on a CVD diamond substrate is proposed. This design offers a highly homogeneous magnetic field, full integration with the diamond substrate, scalability, miniaturization, and efficient heat dissipation, making it a promising solution for NV magnetometry applications. Experimental results confirm its performance, making it a remarkable advancement in this area.

Light Emission and Conductance Fluctuations in Electrically Driven and Plasmonically Enhanced Molecular Junctions.

Electrically connected and plasmonically enhanced molecular junctions combine the optical functionalities of high field confinement and enhancement (cavity function), and of high radiative efficiency (antenna function) with the electrical functionalities of molecular transport. Such combined optical and electrical probes have proven useful for the fundamental understanding of metal-molecule contacts and contribute to the development of nanoscale optoelectronic devices including ultrafast electronics and nanosensors. Here, we employ a self-assembled metal-molecule-metal junction with a nanoparticle bridge to investigate correlated fluctuations in conductance and tunneling-induced light emission at room temperature. Despite the presence of hundreds of molecules in the junction, the electrical conductance and light emission are both highly sensitive to atomic-scale fluctuations-a phenomenology reminiscent of picocavities observed in Raman scattering and of luminescence blinking from photoexcited plasmonic junctions. Discrete steps in conductance associated with fluctuating emission intensities through the multiple plasmonic modes of the junction are consistent with a finite number of randomly localized, point-like sources dominating the optoelectronic response. Contrasting with these microscopic fluctuations, the overall plasmonic and electronic functionalities of our devices feature long-term survival at room temperature and under an electrical bias of a few volts, allowing for measurements over several months.

Broadband on-chip optical non-reciprocity using phase modulators.

Breaking the reciprocity of light propagation in a nanoscale photonic integrated circuit (PIC) is a topic of intense research, fostered by the promises of this technology in areas ranging from experimental research in classical and quantum optics to high-rate telecommunications and data interconnects. In particular, silicon PICs fabricated in processes compatible with the existing complementary metal-oxide-semiconductor (CMOS) infrastructure have attracted remarkable attention. However, a practical solution for integrating optical isolators and circulators within the current CMOS technology remains elusive. Here, we introduce a new non-reciprocal photonic circuit operating with standard single-mode waveguides or optical fibers. Our design exploits a time-dependent index modulation obtained with conventional phase modulators such as the one widely available in silicon photonics platforms. Because it is based on fully balanced interferometers and does not involve resonant structures, our scheme is also intrinsically broadband. Using realistic parameters we calculate an extinction ratio superior to 20dB and insertion loss below 3dB.

A compact and low loss Y-junction for submicron silicon waveguide.

We designed a compact, low-loss and wavelength insensitive Y-junction for submicron silicon waveguide using finite difference time-domain (FDTD) simulation and particle swarm optimization (PSO), and fabricated the device in a 248 nm complementary metal-oxide-semiconductor (CMOS) compatible process. Measured average insertion loss is 0.28 ± 0.02 dB, uniform across an 8-inch wafer. The device footprint is less than 1.2 µm x 2 µm, an order of magnitude smaller than typical multimode interferometers (MMIs) and directional couplers.

Tuning radiative recombination in Cu-doped nanocrystals via electrochemical control of surface trapping.

The incorporation of copper dopants into II-VI colloidal nanocrystals (NCs) leads to the introduction of intragap electronic states and the development of a new emission feature due to an optical transition which couples the NC conduction band to the Cu-ion state. The mechanism underlying Cu-related emission and specifically the factors that control the branching between the intrinsic and impurity-related emission channels remain unclear. Here, we address this problem by conducting spectro-electrochemical measurements on Cu-doped core/shell ZnSe/CdSe NCs. These measurements indicate that the distribution of photoluminescence (PL) intensity between the intrinsic and the impurity bands as well as the overall PL efficiency can be controlled by varying the occupancy of surface defect sites. Specifically, by activating hole traps under negative electrochemical potential (the Fermi level is raised), we can enhance the Cu band at the expense of band-edge emission, which is consistent with the predominant Cu(2+) character of the dopant ions. Furthermore, we observe an overall PL "brightening" under negative potential and "dimming" under positive potential, which we attribute to changes in the occupancy of the electron trap sites (that is, the degree of their electronic passivation) that control nonradiative losses due to electron surface trapping.

Measurement-induced collective vibrational quantum coherence under spontaneous Raman scattering in a liquid.

Spontaneous vibrational Raman scattering is a ubiquitous form of light-matter interaction whose description necessitates quantization of the electromagnetic field. It is usually considered as an incoherent process because the scattered field lacks any predictable phase relationship with the incoming field. When probing an ensemble of molecules, the question therefore arises: What quantum state should be used to describe the molecular ensemble following spontaneous Stokes scattering? We experimentally address this question by measuring time-resolved Stokes-anti-Stokes two-photon coincidences on a molecular liquid consisting of several sub-ensembles with slightly different vibrational frequencies. When spontaneously scattered Stokes photons and subsequent anti-Stokes photons are detected into a single spatiotemporal mode, the observed dynamics is inconsistent with a statistical mixture of individually excited molecules. Instead, we show that the data are reproduced if Stokes-anti-Stokes correlations are mediated by a collective vibrational quantum, i.e. a coherent superposition of all molecules interacting with light. Our results demonstrate that the degree of coherence in the vibrational state of the liquid is not an intrinsic property of the material system, but rather depends on the optical excitation and detection geometry.

Neuronal growth on high-aspect-ratio diamond nanopillar arrays for biosensing applications.

Monitoring neuronal activity with simultaneously high spatial and temporal resolution in living cell cultures is crucial to advance understanding of the development and functioning of our brain, and to gain further insights in the origin of brain disorders. While it has been demonstrated that the quantum sensing capabilities of nitrogen-vacancy (NV) centers in diamond allow real time detection of action potentials from large neurons in marine invertebrates, quantum monitoring of mammalian neurons (presenting much smaller dimensions and thus producing much lower signal and requiring higher spatial resolution) has hitherto remained elusive. In this context, diamond nanostructuring can offer the opportunity to boost the diamond platform sensitivity to the required level. However, a comprehensive analysis of the impact of a nanostructured diamond surface on the neuronal viability and growth was lacking. Here, we pattern a single crystal diamond surface with large-scale nanopillar arrays and we successfully demonstrate growth of a network of living and functional primary mouse hippocampal neurons on it. Our study on geometrical parameters reveals preferential growth along the nanopillar grid axes with excellent physical contact between cell membrane and nanopillar apex. Our results suggest that neuron growth can be tailored on diamond nanopillars to realize a nanophotonic quantum sensing platform for wide-field and label-free neuronal activity recording with sub-cellular resolution.

Pump-intensity- and shell-thickness-dependent evolution of photoluminescence blinking in individual core/shell CdSe/CdS nanocrystals.

We report a systematic study of photoluminescence (PL) intensity and lifetime fluctuations in individual CdSe/CdS core/shell nanocrystal quantum dots (NQDs) as a function of shell thickness. We show that while at low pump intensities PL blinking in thin-shell (4-7 monolayers, MLs) NQDs can be described by random switching between two states of high (ON) and low (OFF) emissivities, it changes to the regime with a continuous distribution of ON intensity levels at high pump powers. A similar behavior is observed in samples with a medium shell thickness (10-12 MLs) without, however, the PL intensity ever switching to a complete "OFF" state and maintaining ca. 30% emissivity ("gray" state). Further, our data indicate that highly stable, blinking-free PL of thick-shell (15-19 MLs) NQDs ("giant" or g-NQDs) is characterized by nearly perfect Poisson statistics, corresponding to a narrow, shot-noise limited PL intensity distribution. Interestingly, in this case the PL lifetime shortens with increasing pump power and the PL decay may deviate from monoexponential. However, the PL intensity distribution remains shot-noise limited, indicating the absence of significant quantum yield fluctuations at a given pump power intensity during the experimental time window.