Quantum interferometry and pathway selectivity in the nonlinear response of photosynthetic excitons.

We propose a time-frequency resolved spectroscopic technique which employs nonlinear interferometers to study exciton-exciton scattering in molecular aggregates. A higher degree of control over the contributing Liouville pathways is obtained as compared to classical light. We show how the nonlinear response can be isolated from the orders-of-magnitude stronger linear background by either phase matching or polarization filtering. Both arise due to averaging the signal over a large number of noninteracting, randomly oriented molecules. We apply our technique to the Frenkel exciton model which excludes charge separation for the photosystem II reaction center. We show how the sum of the entangled photon frequencies can be used to select two-exciton resonances, while their delay times reveal the single-exciton levels involved in the optical process.

Creating large Fock states and massively squeezed states in optics using systems with nonlinear bound states in the continuum.

The quantization of the electromagnetic field leads directly to the existence of quantum mechanical states, called Fock states, with an exact integer number of photons. Despite these fundamental states being long-understood, and despite their many potential applications, generating them is largely an open problem. For example, at optical frequencies, it is challenging to deterministically generate Fock states of order two and beyond. Here, we predict the existence of an effect in nonlinear optics, which enables the deterministic generation of large Fock states at arbitrary frequencies. The effect, which we call an n-photon bound state in the continuum, is one in which a photonic resonance (such as a cavity mode) becomes lossless when a precise number of photons n is inside the resonance. Based on analytical theory and numerical simulations, we show that these bound states enable a remarkable phenomenon in which a coherent state of light, when injected into a system supporting this bound state, can spontaneously evolve into a Fock state of a controllable photon number. This effect is also directly applicable for creating (highly) squeezed states of light, whose photon number fluctuations are (far) below the value expected from classical physics (i.e., shot noise). We suggest several examples of systems to experimentally realize the effects predicted here in nonlinear nanophotonic systems, showing examples of generating both optical Fock states with large n (n >  10), as well as more macroscopic photonic states with very large squeezing, with over 90% less noise (10 dB) than the classical value associated with shot noise.

Tailoring Single-Electron Emission Distributions in the Time-Energy Phase Space.

The precise characterization and control of single-electron wave functions emitted from a single-electron source are essential for advancing electron quantum optics. Here, we introduce a method for tailoring a single-electron emission distribution using energy filtering, enabling selective control of the distribution under various energy barrier conditions of the filter. The tailored electron is studied by reconstructing its Wigner distribution in the time-energy phase space using the continuous-variable tomography method. Our results reveal that the filtering cuts the portion of the distribution below the energy-barrier height of the filter in the time-energy space. While the filtering is demonstrated in a classical regime of the emitted electrons, we expect that this study significantly contributes to the design and implementation of advanced experiments toward quantum information processing based on single electrons.

Purcell-Induced Bright Single Photon Emitters in Hexagonal Boron Nitride.

Single photon emitters (SPEs) in hexagonal boron nitride (hBN) are elementary building blocks for room-temperature on-chip quantum photonic technologies. However, fundamental challenges, such as slow radiative decay and nondeterministic placement of the emitters, limit their full potential. Here, we demonstrate large-area arrays of plasmonic nanoresonators (PNRs) for Purcell-induced room-temperature SPEs by engineering emitter-cavity coupling and enhancing radiative emission. Gold-coated silicon pillars with an alumina spacer enable a 10-fold local-field enhancement in the emission band of native hBN defects. We observe bright SPEs with an average saturated emission rate surpassing 5 million counts per second, an average lifetime of <0.5 ns, and 29% yield. Density functional theory reveals the beneficial role of an alumina spacer between hBN and gold, mitigating the electronic broadening of emission from defects proximal to the metal. Our results offer arrays of bright, heterogeneously integrated single-photon sources, paving the way for robust and scalable quantum information systems.

Control of Quantized Spontaneous Emission from Single GaAs Quantum Dots Embedded in Huygens' Metasurfaces.

Advancements in photonic quantum information systems (QIS) have driven the development of high-brightness, on-demand, and indistinguishable semiconductor epitaxial quantum dots (QDs) as single photon sources. Strain-free, monodisperse, and spatially sparse local-droplet-etched (LDE) QDs have recently been demonstrated as a superior alternative to traditional Stranski-Krastanov QDs. However, integration of LDE QDs into nanophotonic architectures with the ability to scale to many interacting QDs is yet to be demonstrated. We present a potential solution by embedding isolated LDE GaAs QDs within an Al0.4Ga0.6As Huygens' metasurface with spectrally overlapping fundamental electric and magnetic dipolar resonances. We demonstrate for the first time a position- and size-independent, 1 order of magnitude increase in the collection efficiency and emission lifetime control for single-photon emission from LDE QDs embedded within the Huygens' metasurfaces. Our results represent a significant step toward leveraging the advantages of LDE QDs within nanophotonic architectures to meet the scalability demands of photonic QIS.

Continuously tunable single-photon level nonlinearity with Rydberg state wave-function engineering.

Extending optical nonlinearity into the extremely weak light regime is at the heart of quantum optics, since it enables the efficient generation of photonic entanglement and implementation of photonic quantum logic gate. Here, we demonstrate the capability for continuously tunable single-photon level nonlinearity, enabled by precise control of Rydberg interaction over two orders of magnitude, through the use of microwave-assisted wave-function engineering. To characterize this nonlinearity, light storage and retrieval protocol utilizing Rydberg electromagnetically induced transparency is employed, and the quantum statistics of the retrieved photons are analyzed. As a first application, we demonstrate our protocol can speed up the preparation of single photons in low-lying Rydberg states by a factor of up to∼40. Our work holds the potential to accelerate quantum operations and to improve the circuit depth and connectivity in Rydberg systems, representing a crucial step towards scalable quantum information processing with Rydberg atoms.

Nano antenna-assisted quantum dots emission into high-index planar waveguide.

Integrated quantum photonic circuits require the efficient coupling of photon sources to photonic waveguides. Hybrid plasmonic/photonic platforms are a promising approach, taking advantage of both plasmon modal confinement for efficient coupling to a nearby emitter and photonic circuitry for optical data transfer and processing. In this work, we established directional quantum dot (QD) emission coupling to a planar TiO2waveguide assisted by a Yagi-Uda antenna. Antenna on waveguide is first designed by scaling radio frequency dimensions to nano-optics, taking into account the hybrid plasmonic/photonic platform. Design is then optimized by full numerical simulations. We fabricate the antenna on a TiO2planar waveguide and deposit a few QDs close to the Yagi-Uda antenna. The optical characterization shows clear directional coupling originating from antenna effect. We estimate the coupling efficiency and directivity of the light emitted into the waveguide.

A High-Finesse Suspended Interferometric Sensor for Macroscopic Quantum Mechanics with Femtometre Sensitivity.

We present an interferometric sensor for investigating macroscopic quantum mechanics on a table-top scale. The sensor consists of a pair of suspended optical cavities with finesse over 350,000 comprising 10 g fused silica mirrors. The interferometer is suspended by a four-stage, light, in-vacuum suspension with three common stages, which allows for us to suppress common-mode motion at low frequency. The seismic noise is further suppressed by an active isolation scheme, which reduces the input motion to the suspension point by up to an order of magnitude starting from 0.7 Hz. In the current room-temperature operation, we achieve a peak sensitivity of 0.5 fm/Hz in the acoustic frequency band, limited by a combination of readout noise and suspension thermal noise. Additional improvements of the readout electronics and suspension parameters will enable us to reach the quantum radiation pressure noise. Such a sensor can eventually be utilized for demonstrating macroscopic entanglement and for testing semi-classical and quantum gravity models.

Quantum Photonic Circuits Integrated with Color Centers in Designer Nanodiamonds.

Diamond has emerged as a leading host material for solid-state quantum emitters, quantum memories, and quantum sensors. However, the challenges in fabricating photonic devices in diamond have limited its potential for use in quantum technologies. While various hybrid integration approaches have been developed for coupling diamond color centers with photonic devices defined in a heterogeneous material, these methods suffer from either large insertion loss at the material interface or evanescent light-matter coupling. Here, we present a new technique that enables the deterministic assembly of diamond color centers in a silicon nitride photonic circuit. Using this technique, we observe Purcell enhancement of silicon vacancy centers coupled to a silicon nitride ring resonator. Our hybrid integration approach has the potential for achieving the maximum possible light-matter interaction strength while maintaining low insertion loss and paves the way toward scalable manufacturing of large-scale quantum photonic circuits integrated with high-quality quantum emitters and spins.

Electric-Field Fluctuations as the Cause of Spectral Instabilities in Colloidal Quantum Dots.

Spectral diffusion (SD) represents a substantial obstacle toward implementation of solid-state quantum emitters as a source of indistinguishable photons. By performing high-resolution emission spectroscopy for individual colloidal quantum dots at cryogenic temperatures, we prove the causal link between the quantum-confined Stark effect and SD. Statistically analyzing the wavelength of emitted photons, we show that increasing the sensitivity of the transition energy to an applied electric field results in amplified spectral fluctuations. This relation is quantitatively fit to a straightforward model, indicating the presence of a stochastic electric field on a microscopic scale, whose standard deviation is 9 kV/cm, on average. The current method will enable the study of SD in multiple types of quantum emitters such as solid-state defects or organic lead halide perovskite quantum dots, for which spectral instability is a critical barrier for applications in quantum sensing.

Beyond the Four-Level Model: Dark and Hot States in Quantum Dots Degrade Photonic Entanglement.

Entangled photon pairs are essential for a multitude of quantum photonic applications. To date, the best performing solid-state quantum emitters of entangled photons are semiconductor quantum dots operated around liquid-helium temperatures. To favor the widespread deployment of these sources, it is important to explore and understand their behavior at temperatures accessible with compact Stirling coolers. Here we study the polarization entanglement among photon pairs from the biexciton-exciton cascade in GaAs quantum dots at temperatures up to ∼65 K. We observe entanglement degradation accompanied by changes in decay dynamics, which we ascribe to thermal population and depopulation of hot and dark states in addition to the four levels relevant for photon pair generation. Detailed calculations considering the presence and characteristics of the additional states and phonon-assisted transitions support the interpretation. We expect these results to guide the optimization of quantum dots as sources of highly entangled photons at elevated temperatures.

On-Chip Electrostatic Actuation of a Photonic Wire Antenna Embedding Quantum Dots.

A photonic wire antenna embedding individual quantum dots (QDs) constitutes a promising platform for both quantum photonics and hybrid nanomechanics. We demonstrate here an integrated device in which on-chip electrodes can apply a static or oscillating bending force to the upper part of the wire. In the static regime, we achieve control over the bending direction and apply at will tensile or compressive mechanical stress on any QD. This results in a blue shift or red shift of their emission, with direct application to the realization of broadly tunable sources of quantum light. As a first illustration of operation in the dynamic regime, we excite the wire fundamental flexural mode and use the QD emission to detect the mechanical vibration. With an estimated operation bandwidth in the GHz range, electrostatic actuation opens appealing perspectives for the exploration of QD-nanowire hybrid mechanics with high-frequency vibrational modes.

The controversy about interference of photons.

In the 1960s, the demonstration of interference effects using two laser-beams raised the question: can two photons interfere? Its plausibility contested Dirac's dictum, "Interference between two different photons never occurs". Disagreements about this conflict led to a controversy. This paper will chart the controversy's contour and show that it evolved over two phases. Subsequently, I investigate the reasons for its perpetuation. The controversy was initiated and fuelled by several misinterpretations of the dictum. I also argue that Dirac's dictum is not applicable to two photon interference as they belong to different contexts of interference. Recognising this resolves the controversy.

Strong-laser-field physics, non-classical light states and quantum information science.

Strong-laser-field physics is a research direction that relies on the use of high-power lasers and has led to fascinating achievements ranging from relativistic particle acceleration to attosecond science. On the other hand, quantum optics has been built on the use of low photon number sources and has opened the way for groundbreaking discoveries in quantum technology, advancing investigations ranging from fundamental tests of quantum theory to quantum information processing. Despite the tremendous progress, until recently these directions have remained disconnected. This is because the majority of the interactions in the strong-field limit have been successfully described by semi-classical approximations treating the electromagnetic field classically, as there was no need to include the quantum properties of the field to explain the observations. The link between strong-laser-field physics, quantum optics, and quantum information science has been developed in the recent past. Studies based on fully quantized and conditioning approaches have shown that intense laser-matter interactions can be used for the generation of controllable entangled and non-classical light states. These achievements open the way for a vast number of investigations stemming from the symbiosis of strong-laser-field physics, quantum optics, and quantum information science. Here, after an introduction to the fundamentals of these research directions, we report on the recent progress in the fully quantized description of intense laser-matter interaction and the methods that have been developed for the generation of non-classical light states and entangled states. Also, we discuss the future directions of non-classical light engineering using strong laser fields, and the potential applications in ultrafast and quantum information science.

Coupling of light and mechanics in a photonic crystal waveguide.

Observations of thermally driven transverse vibration of a photonic crystal waveguide (PCW) are reported. The PCW consists of two parallel nanobeams whose width is modulated symmetrically with a spatial period of 370 nm about a 240-nm vacuum gap between the beams. The resulting dielectric structure has a band gap (i.e., a photonic crystal stop band) with band edges in the near infrared that provide a regime for transduction of nanobeam motion to phase and amplitude modulation of an optical guided mode. This regime is in contrast to more conventional optomechanical coupling by way of moving end mirrors in resonant optical cavities. Models are developed and validated for this optomechanical mechanism in a PCW for probe frequencies far from and near to the dielectric band edge (i.e., stop band edge). The large optomechanical coupling strength predicted should make possible measurements with an imprecision below that at the standard quantum limit and well into the backaction-dominated regime. Since our PCW has been designed for near-field atom trapping, this research provides a foundation for evaluating possible deleterious effects of thermal motion on optical atomic traps near the surfaces of PCWs. Longer-term goals are to achieve strong atom-mediated links between individual phonons of vibration and single photons propagating in the guided modes (GMs) of the PCW, thereby enabling optomechanics at the quantum level with atoms, photons, and phonons. The experiments and models reported here provide a basis for assessing such goals.

Experimental Guesswork with Quantum Side Information Using Twisted Light.

Guesswork is an information-theoretic quantity which can be seen as an alternate security criterion to entropy. Recent work has established the theoretical framework for guesswork in the presence of quantum side information, which we extend both theoretically and experimentally. We consider guesswork when the side information consists of the BB84 states and their higher-dimensional generalizations. With this side information, we compute the guesswork for two different scenarios for each dimension. We then performed a proof-of-principle experiment using Laguerre-Gauss modes to experimentally compute the guesswork for higher-dimensional generalizations of the BB84 states. We find that our experimental results agree closely with our theoretical predictions. This work shows that guesswork can be a viable security criterion in cryptographic tasks and is experimentally accessible in a number of optical setups.

Purcell Enhancement of Erbium Ions in TiO2 on Silicon Nanocavities.

Isolated solid-state atomic defects with telecom optical transitions are ideal quantum photon emitters and spin qubits for applications in long-distance quantum communication networks. Prototypical telecom defects, such as erbium, suffer from poor photon emission rates, requiring photonic enhancement using resonant optical cavities. Moreover, many of the traditional hosts for erbium ions are not amenable to direct incorporation with existing integrated photonics platforms, limiting scalable fabrication of qubit-based devices. Here, we present a scalable approach toward CMOS-compatible telecom qubits by using erbium-doped titanium dioxide thin films grown atop silicon-on-insulator substrates. From this heterostructure, we have fabricated one-dimensional photonic crystal cavities demonstrating quality factors in excess of 5 × 104 and corresponding Purcell-enhanced optical emission rates of the erbium ensembles in excess of 200. This easily fabricated materials platform represents an important step toward realizing telecom quantum memories in a scalable qubit architecture compatible with mature silicon technologies.

Donor-Acceptor Pair Quantum Emitters in Hexagonal Boron Nitride.

Quantum emitters are needed for a myriad of applications ranging from quantum sensing to quantum computing. Hexagonal boron nitride (hBN) quantum emitters are one of the most promising solid-state platforms to date due to their high brightness and stability and the possibility of a spin-photon interface. However, the understanding of the physical origins of the single-photon emitters (SPEs) is still limited. Here we report dense SPEs in hBN across the entire visible spectrum and present evidence that most of these SPEs can be well explained by donor-acceptor pairs (DAPs). On the basis of the DAP transition generation mechanism, we calculated their wavelength fingerprint, matching well with the experimentally observed photoluminescence spectrum. Our work serves as a step forward for the physical understanding of SPEs in hBN and their applications in quantum technologies.

One-Lead Single-Electron Source with Charging Energy.

Single-electron sources, formed by a quantum dot (QD), are key elements for realizing electron analogue of quantum optics. We develop a new type of single-electron source with functionalities that are absent in existing sources. This source couples with only one lead. By an AC rf drive, it successively emits holes and electrons cotraveling in the lead, as in the mesoscopic capacitor. Thanks to the considerable charging energy of the QD, however, emitted electrons have energy levels a few tens of millielectronvolts above the Fermi level, so that emitted holes and electrons are split by a potential barrier on demand, resulting in a rectified quantized current. The resulting pump map exhibits quantized triangular islands, in good agreement with our theory. We also demonstrate that the source can be operated with another tunable-barrier single-electron source in a series double QD geometry, showing parallel electron pumping by a common gate driving.

Clocked atom delivery to a photonic crystal waveguide.

Experiments and numerical simulations are described that develop quantitative understanding of atomic motion near the surfaces of nanoscopic photonic crystal waveguides (PCWs). Ultracold atoms are delivered from a moving optical lattice into the PCW. Synchronous with the moving lattice, transmission spectra for a guided-mode probe field are recorded as functions of lattice transport time and frequency detuning of the probe beam. By way of measurements such as these, we have been able to validate quantitatively our numerical simulations, which are based upon detailed understanding of atomic trajectories that pass around and through nanoscopic regions of the PCW under the influence of optical and surface forces. The resolution for mapping atomic motion is roughly 50 nm in space and 100 ns in time. By introducing auxiliary guided-mode (GM) fields that provide spatially varying AC Stark shifts, we have, to some degree, begun to control atomic trajectories, such as to enhance the flux into the central vacuum gap of the PCW at predetermined times and with known AC Stark shifts. Applications of these capabilities include enabling high fractional filling of optical trap sites within PCWs, calibration of optical fields within PCWs, and utilization of the time-dependent, optically dense atomic medium for novel nonlinear optical experiments.