Second-order Correlation Research Articles

Defogging imaging using second-order correlations in the time domain

The traditional space-domain McCartney model simplifies fog as a time-invariant medium, as the fluctuation of light field introduced by time-varying fog is a noise for optical imaging. Here, an opposite finding to traditional idea is reported, i.e., the noise introduced by time-varying fog can be eliminated by itself. The space-time McCartney model is proposed to study the second-order correlations of the time-varying scattering light field in the time domain. We theoretically and experimentally demonstrate that the noise photons, which cause image degradation, lead to the absence of stable second-order correlations, while the signal photons, which produce ideal images, are opposite. The noise photons and signal photons are distinguished by measuring the temporal second-order correlations when fog is time-varying and time interval is longer than the coherence time of the light field, thereby reconstructing high-quality defogging images. Distinguishable images can be directly obtained even when the target is indistinguishable by conventional cameras, providing a prerequisite for subsequent high-level computer vision tasks. The space-time McCartney model provides a theoretical framework for studying the light field properties of time-varying media, and offers promise for anti-interference imaging.

Photon blockade in a double-transmon system with ultrastrong coupling

The circuit quantum electrodynamics (QED) system has brought us into an ultrastrong and deep coupling regime in the light–matter interaction community, in which the quantum effect has attracted significant interest. In this study, we theoretically investigated the photon blockade phenomenon in a double-transmon system operating in an ultrastrong coupling regime. We considered the effect of the counter-rotating wave terms in the interaction Hamiltonian and derived the master equation in the eigenpresentation. We found that photon blockade occurred in only one of the eigenmodes, and the counter-rotating wave terms enhanced the blockade by reducing the minimum value of the second-order correlation function. This study will be beneficial for the design of single-photon devices in circuit QED systems, especially in the ultrastrong coupling regime.

Photon blockade in a high-damping cavity via a gain-type coupler

Abstract We propose a scheme to implement photon blockade in a non-Hermitian circuit quantum electrodynamics (circuit-QED) system where a single-mode cavity interacts with a two-level emitter through virtual photon excitation mediated by a coupler resonator. A damping compensation regime is introduced by the phase-lag arising from the medium mode, thereby the periodic exceptional points (EPs) are observed at which the system achieves gain-damping balance. This regime enables photon blockade to occur within the single-mode cavity with high-damping rate by controlling the gain circuit of the coupler, which breaks the limitation of a low-damping rate for photon blockade under weak drive and relaxes the stringent requirements on the quality factor of the cavity. The numerical simulations for the second-order correlation function, obtained using reported experimental parameters, exhibit excellent agreement with our analytical results. The findings of this study provide a circuit-QED solution for single-quantum devices based on the high-damping cavities, which is of great significance for integrated quantum computing networks.

Rain-free imaging using second-order correlations in the time domain

Rain-free imaging using second-order correlations in the time domain

Versatile VCSEL source of thermal and super-thermal light.

We have built highly controllable sources of thermal and super-thermal states on the basis of a single-mode (SM) and a multi-mode (MM) vertical cavity surface emitting laser (VCSEL) with noised driving current operating above the threshold. Varying the average driving current and the amplitude and bandwidth of noise, one can robustly obtain light with the temporal second-order intensity correlation function reaching 2.5 and correlation times from 1 µs to 10 ns. For the SM VCSEL, generated thermal lights retain its single-mode quality negating a need for a spectral filtering. For the MM VCSEL, one can still find a near-threshold regime when the generated thermal radiation is close to a single-mode one.

Third-order intrinsic alignment of SDSS BOSS LOWZ galaxies

Cosmic shear is a powerful probe of cosmology, but it is affected by the intrinsic alignment (IA) of galaxy shapes with the large-scale structure. Upcoming surveys such as Euclid and Vera C. Rubin Observatory's Legacy Survey of Space and Time (LSST) require an accurate understanding of IA, particularly for higher-order cosmic shear statistics that are vital for extracting the most cosmological information. In this paper, we report the first detection of third-order IA correlations using the LOWZ galaxy sample from the Sloan Digital Sky Survey (SDSS) Baryon Oscillation Spectroscopic Survey (BOSS). We compare our measurements with predictions from the MICE cosmological simulation and an analytical model inspired by the Non-linear Linear Alignment (NLA) model and informed by second-order correlations. We also explore the dependence of the third-order correlation on the galaxies' luminosity. We find that the amplitude $A_ IA $ of the IA signal is non-zero at the $4.7 level for scales between Mpc Mpc Mpc Mpc $ the inferred $A_ IA $ agrees both with the prediction from the simulation and estimates from second-order statistics within 1sigma but deviations arise at smaller scales. Our results demonstrate the feasibility of measuring third-order IA correlations and using them for constraining IA models. The agreement between second- and third-order IA constraints also opens the opportunity for a consistent joint analysis and IA self-calibration, promising tighter parameter constraints for upcoming cosmological surveys.

Orchestrating time and color: a programmable source of high-dimensional entanglement

High-dimensional encodings based on temporal modes (TMs) of photonic quantum states provide the foundations for a highly versatile and efficient quantum information science (QIS) framework. Here, we demonstrate a crucial building block for any QIS applications based on TMs: a programmable source of maximally entangled high-dimensional TM states. Our source is based on a parametric downconversion process driven by a spectrally shaped pump pulse, which facilitates the generation of maximally entangled TM states with a well-defined dimensionality that can be chosen programmatically. We characterize the effective dimensionality of the generated states via measurements of second-order correlation functions and joint spectral intensities, demonstrating the generation of bi-photon TM states with a controlled dimensionality in up to 20 dimensions.

Noiselessly amplified thermal states and after multi-photon addition or subtraction

In this paper, we study the combined effects of the ideal amplification operator ([Formula: see text]) and m-photon added operator [Formula: see text] (or m-photon subtracted operator [Formula: see text]) on the thermal state ([Formula: see text]), with mean photon number (MPN [Formula: see text]). By only operating [Formula: see text] on [Formula: see text], we introduce a noiselessly amplified thermal state (ATS [Formula: see text]) with larger MPN [Formula: see text]. The selection of [Formula: see text] and g must ensure that the process is physical ([Formula: see text]). By operating [Formula: see text] and [Formula: see text] (or [Formula: see text]) on [Formula: see text] successively, we further introduce photon-added-ATS (ρ m+) or photon-subtracted-ATS (ρ m−). Then, we analyze their photon number distributions and prove that the purity of ρ m+ is equal to that of ρ m−. Meanwhile, we study their nonclassicality by examing Mandel parameter and second-order correlation function. Finally, we study their three quasiprobability distributions, whose negativities are other signatures of the nonclassicality. Our study demonstrates that photon addition has more pronounced effects on nonclassicality than photon subtraction. Our study will provide useful theoretical references for experiments and applications.

Quantum tunneling high-speed nano-excitonic modulator

High-speed electrical control of nano-optoelectronic properties in two-dimensional semiconductors is a building block for the development of excitonic devices, allowing the seamless integration of nano-electronics and -photonics. Here, we demonstrate a high-speed electrical modulation of nanoscale exciton behaviors in a MoS2 monolayer at room temperature through a quantum tunneling nanoplasmonic cavity. Electrical control of tunneling electrons between Au tip and MoS2 monolayer facilitates the dynamic switching of neutral exciton- and trion-dominant states at the nanoscale. Through tip-induced spectroscopic analysis, we locally characterize the modified recombination dynamics, resulting in a significant change in the photoluminescence quantum yield. Furthermore, by obtaining a time-resolved second-order correlation function, we demonstrate that this electrically-driven nanoscale exciton-trion interconversion achieves a modulation frequency of up to 8 MHz. Our approach provides a versatile platform for dynamically manipulating nano-optoelectronic properties in the form of transformable excitonic quasiparticles, including valley polarization, recombination, and transport dynamics.

Characterizing Rotational Dynamics and Heterogeneity via Single-Molecule Intensity Measurements.

Dynamic heterogeneity in glassy systems has typically been characterized at the single-molecule level by extracting rotational relaxation time scales from linear dichroism (LD) collected via two orthogonally polarized channels. However, in such measurements, localization precision is diminished due to photons lost relative to collection in a single detection channel. This poses challenges in characterizing rotational and translational dynamics simultaneously, as translational measurements require high localization precision. In this paper, we present a method for extracting rotational dynamics of glassy systems at the single-molecule level from intensity fluctuations of fluorescent probe molecules in a wide-field configuration without the use of a polarizing optical component. Through numerical analysis, we show that LD and intensity measurements probing rotational dynamics report similar, approximately second-order rotational correlation decays even at low signal to noise. Thus, within the assumptions of small, isotropic rotations, LD and intensity autocorrelation analysis should provide identical information on the time scale and heterogeneity of rotational dynamics. We then present experimental results that validate this numerical result, with direct comparison of LD and intensity-based approaches across probe molecules in both polymeric and small-molecule glass formers as well as across optical configurations. Our results demonstrate moderate correlation on a per-probe basis between rotational time scales obtained from both approaches, with deviations consistent with those expected in a dynamically heterogeneous system. We envision that this easily accessible strategy will be of use across disciplines for characterizing single-molecule rotational dynamics in limited signal situations and/or when high-precision localization is required.

Sediment microbial fuel cells capable of powering outdoor environmental monitoring sensors

In this study, Sediment Microbial Fuel Cells (SMFCs) prototypes have been developed to operate under open-air conditions and power sensors for environmental monitoring. Two SMFCs with a volume of 50 l each, consisting of two types of anodic materials – graphite and coke, were operated on-field for over a year. The electrical outputs have been recorded and compared with the measured environmental parameters such as temperature, light illumination, atmospheric pressure, humidity, etc. The statistical analysis of the obtained data shows that temperature changes between 0 and 14 °C do not affect the power achieved. On the contrary, the sunlight irradiation showed a second-order polynomial correlation with the current generated by the SMFCs, increasing the latter during the days. The cathode reactions significantly impacted the power density achieved by both explored SMFCs and the system's sustainability. The metallurgical coke is suggested to be used as an inexpensive and convenient anode material for SMFCs giving compatible results to the widely used graphite.

Optimized higher-order photon state classification by machine learning

The classification of higher-order photon emission becomes important with more methods being developed for deterministic multiphoton generation. The widely used second-order correlation g(2) is not sufficient to determine the quantum purity of higher photon Fock states. Traditional characterization methods require a large amount of photon detection events, which leads to increased measurement and computation time. Here, we demonstrate a machine learning model based on a 2D Convolutional Neural Network (CNN) for rapid classification of multiphoton Fock states up to |3⟩ with an overall accuracy of 94%. By fitting the g(3) correlation with simulated photon detection events, the model exhibits an efficient performance particularly with sparse correlation data, with 800 co-detection events to achieve an accuracy of 90%. Using the proposed experimental setup, this CNN classifier opens up the possibility for quasi-real-time classification of higher photon states, which holds broad applications in quantum technologies.

Quantum dual-path interferometry scheme for axion dark matter searches

Exploring the mysterious dark matter is a key quest in modern physics. Currently, detecting axions, a hypothetical particle proposed as a primary component of dark matter, remains a significant challenge due to their weakly interacting nature. Here we show at quantum level that in a cavity permeated by a magnetic field, the single axion-photon conversion rate is enhanced by the cavity quality factor and is quantitatively larger than the classical result by π/2. The axion cavity can be considered a quantum device emitting single photons with temporal separations. This differs from the classical picture and reveals a possibility for the axion cavity experiment to handle the signal sensitivity at the quantum level, e.g., a dual path quantum interferometry with cross-power and second-order correlation measurements. This scheme would greatly reduce the signal scanning time and improve the sensitivity of the axion-photon coupling, potentially leading to the direct observation of axions.

(Invited) Correlation Measurements for Carbon Nanotubes with Quantum Defects

Single-photon sources are one of the essential building blocks for the development of photonic quantum technology. In terms of potential practical application, an on-demand electrically driven quantum-light emitter on a chip is notably crucial for integrating photonic integrated circuits. Here, we propose functionalized single-walled carbon nanotube field-effect transistors as a promising solid-state quantum-light source by demonstrating photon antibunching behavior via electrical excitation. The sp3 quantum defects were formed on the surface of (7, 5) carbon nanotubes by 3,5-dichlorophenyl functionalization, and individual carbon nanotubes were wired to graphene electrode pairs. Filtered electroluminescent defect-state emission at 77 K was coupled into a Hanbury Brown and Twiss experiment setup, and single-photon emission was observed by performing second-order correlation function measurements. We discuss the dependence of the intensity correlation measurement on excitation power and emission wavelength highlighting the challenges of performing such measurements while simultaneously analyzing acquired data. Our results indicate a route toward room-temperature electrically-triggered single-photon emission.

(Invited) Photoluminescence Properties of Single InAsP Quantum Dots Embedded in InP Nanowires

Non-classical light emitters that can generate single photons with a negligible multiphoton probability are one of the key components for quantum information technologies. Deterministically grown III-V semiconductor nanowires containing quantum dots are gaining interest as a viable platform for quantum key distribution applications. In this talk, we will report on our recent development of the fabrication of InAsP single quantum dots embedded within InP photonic waveguide nanowires. In particular, we outline the importance of the photonic waveguide design for optimum photon generation and coupling to external optics [1]. The measured count rate dependence on normalized wire diameter, D/λ (figure 1) of the nanowire sources is consistent with calculations of the spontaneous emission rate into the fundamental HE11 nanowire waveguide mode (ΓHE11). Manipulating dot growth conditions and engineering the band structure around the dot (dot-in-a-rod configuration) are applied [2] to enhance the photoluminescence emission rate at 1310 nm and 1550 nm. Single photon emission with very low multiple photon probability is demonstrated at O- and C-band [3,4]. Temperature dependent, second-order correlation measurements on the 1310 nm source show that these nanowire sources can generate single photons up to temperatures of 220 K [3].[1] S. Haffouz, et al., Nano Letters, 18, 3047 (2018).[2] S. Haffouz, et al., Applied Physics Letters, 117, 113101 (2020).[3] P. Laferriére, et al., Nano Letters, 23, 962 (2023).[4] A.N. Wakileh, et al., arXiv:2309.13381 (2023). Figure 1

3D Correlation Imaging for Localized Phase Disturbance Mitigation

Correlation plenoptic imaging is a procedure to perform light-field imaging without spatial resolution loss, by measuring the second-order spatiotemporal correlations of light. We investigate the possibility of using correlation plenoptic imaging to mitigate the effect of a phase disturbance in the propagation from the object to the main lens. We assume that this detrimental effect, which can be due to a turbulent medium, is localized at a specific distance from the lens, and is slowly varying in time. The mitigation of turbulence effects has already fostered the development of both light-field imaging and correlation imaging procedures. Here, we aim to merge these aspects, proposing a correlation light-field imaging method to overcome the effects of slowly varying turbulence, without the loss of lateral resolution, typical of traditional plenoptic imaging devices.

Advanced analysis of single-molecule spectroscopic data

We present Full SMS, a multipurpose graphical user interface (GUI)-based software package for analyzing single-molecule spectroscopy (SMS) data. SMS typically delivers multiparameter data—such as fluorescence brightness, lifetime, and spectra—of molecular- or nanometer-scale particles such as single dye molecules, quantum dots, or fluorescently labeled biological macromolecules. Full SMS allows an unbiased statistical analysis of fluorescence brightness through level resolution and clustering, analysis of fluorescence lifetimes through decay fitting, as well as the calculation of second-order correlation functions and the display of fluorescence spectra and raster-scan images. Additional features include extensive data filtering options, a custom HDF5-based file format, and flexible data export options. The software is open source and written in Python but GUI based so it may be used without any programming knowledge. A multiprocess architecture was employed for computational efficiency. The software is also designed to be easily extendable to include additional import data types and analysis capabilities.

Silent white light: Reduction of the second-order intensity correlation coefficient

We investigate the intrawaveguide statistics manipulation of broadband light by combining semiconductor quantum dot physics with quantum optics. By cooling a quantum dot superluminescent diode to the liquid nitrogen temperature of 77 K, Blazek [] have demonstrated a temperature-dependent reduction of the second-order intensity correlation coefficient from 2 for thermal amplified spontaneous emission light to g(2)(0,T=190K)≈1.33. Here, we model the broadband photon statistics assuming amplified spontaneous emission radiation in a pumped, saturable quantum dot gain medium. We demonstrate that, by an intensity increase due to the quantum dot occupation dynamics via the temperature-tuned quasi-Fermi levels, together with the saturation nonlinearity, a statistics manipulation from thermal Bose-Einstein statistics towards Poissonian statistics can be realized, thus producing “silent white light” with a reduced second-order correlation coefficient. Such intensity-noise-reduced broadband radiation is relevant for many applications such as optical coherence tomography, optical communication, or optical tweezers. Published by the American Physical Society 2024

Colossal Core/Shell CdSe/CdS Quantum Dot Emitters.

Single-photon sources are essential for advancing quantum technologies with scalable integration being a crucial requirement. To date, deterministic positioning of single-photon sources in large-scale photonic structures remains a challenge. In this context, colloidal quantum dots (QDs), particularly core/shell configurations, are attractive due to their solution processability. However, traditional QDs are typically small, about 3 to 6 nm, which restricts their deterministic placement and utility in large-scale photonic devices, particularly within optical cavities. The largest existing core/shell QDs are a family of giant CdSe/CdS QDs, with total diameters ranging from about 20 to 50 nm. Pushing beyond this size limit, we introduce a synthesis strategy for colossal CdSe/CdS QDs, with sizes ranging from 30 to 100 nm, using a stepwise high-temperature continuous injection method. Electron microscopy reveals a consistent hexagonal diamond morphology composed of 12 semipolar {101̅1} facets and one polar (0001) facet. We also identify conditions where shell growth is disrupted, leading to defects, islands, and mechanical instability, which suggest synthetic requirements for growing crystalline particles beyond 100 nm. The stepwise growth of thick CdS shells on CdSe cores enables the synthesis of emissive QDs with long photoluminescence lifetimes of a few microseconds and suppressed blinking at room temperature. Notably, QDs with 80 and 100 CdS monolayers exhibit high single-photon emission purity with second-order photon correlation g(2)(0) values below 0.2.

Realization of nonreciprocal photon statistics by manipulating the quantum nonlinearity of cold atoms in an asymmetric cavity.

In a strongly coupled cavity quantum electrodynamics (QED) system, the second-order correlation function g(2)(τ) of the transmitted probe light from the cavity is determined by the nonlinearity of the atom in the cavity. Therefore, the system provides a platform for controlling the photon statistics by manipulating nonlinearity. In this paper, we experimentally demonstrate nonreciprocal quantum statistics in a cavity QED system with several atoms strongly coupled to an asymmetric optical cavity, which is composed of two mirrors with different transmittivities. When the direction of the probe light is reversed, the intracavity light field alternates to a different level. Distinct photon statistics are then observed due to the quantum nonlinearity associated with strongly coupled atoms. Sub-Poissonian photon-number statistics for forward light and a Poissonian distribution for backward light are then realized. Our work provides an effective approach for realizing nonreciprocal quantum devices, which have potential applications in the unidirectional generation of nonclassical light fields and quantum sensing.