Photoacoustic Heterodyne CO Sensor for Rapid Detection of CO Impurities in Hydrogen.

Hydrogen (H2) fuel cells have been developed as an environmentally benign, low-carbon, and efficient energy option in the current period of promoting low-carbon activities, which offer a compelling means to reduce carbon emissions. However, the presence of carbon monoxide (CO) impurities in H2 may potentially damage the fuel cell's anode. As a result, monitoring of the CO levels in fuel cells has become a significant area of research. In this paper, a novel photoacoustic sensor is developed based on photoacoustic heterodyne technology. The sensor combines a 4.61 µm mid-infrared quantum cascade laser with a low-noise differential photoacoustic cell. This combination enables fast, real-time online detection of CO impurity concentrations in H2. Notably, the sensor requires no wavelength locking to monitor CO online in real-time and produces a single effective signal with a period of only 15 ms. Furthermore, the sensor's performance was thoroughly evaluated in terms of detection sensitivity, linearity, and long-term stability. The minimum detection limit of 11 ppb was obtained at an optimal time constant of 1 s.

Conversion of Photoluminescence Blinking Types in Single Colloidal Quantum Dots.

Almost all colloidal quantum dots (QDs) exhibit undesired photoluminescence (PL) blinking, which poses a significant obstacle to their use in numerous luminescence applications. An in-depth study of the blinking behavior, along with the associated mechanisms, can provide critical opportunities for fabricating high-quality QDs for diverse applications. Here the blinking of a large series of colloidal QDs is investigated with different surface ligands, particle sizes, shell thicknesses, and compositions. It is found that the blinking behavior of single alloyed CdSe/ZnS QDs with a shell thickness of up to 2 nm undergoes an irreversible conversion from Auger-blinking to band-edge carrier blinking (BC-blinking). Contrastingly, single perovskite QDs with particle sizes smaller than their Bohr diameters exhibit reversible conversion between BC-blinking and more pronounced Auger-blinking. Changes in the effective trapping sites under different excitation conditions are found to be responsible for the blinking type conversions. Additionally, changes in shell thickness and particle size of QDs have a significant effect on the blinking type conversions due to altered wavefunction overlap between excitons and effective trapping sites. This study elucidates the discrepancies in the blinking behavior of various QD samples observed in previous reports and provides deeper understanding of the mechanisms underlying diverse types of blinking.

Microwave coupled Zeeman splitting spectroscopy of a cesium nPJ Rydberg atom.

We perform measurements of microwave spectra of cesium Rydberg 51S1/2 → 51PJ transitions with the linewidth approaching the Fourier limit. A two-photon scheme excites the ground-state atoms to the Rydberg 51S1/2 state, and a weak microwave photon couples the Rydberg transition of 51S1/2 → 51PJ. The hyperfine structure of 51P1/2 can be clearly resolved with a narrow linewidth microwave spectra by using the method of ion detection. Furthermore, we investigate the Zeeman effect of the 51P1/2,3/2 state. The theoretical calculations reproduce the measurement well. Our experimental measurements provide a reliable technical solution for the investigation of high angular momentum Rydberg states, which is conducive to further realizing the coherent manipulation of Rydberg energy levels and improving the sensitivity of electromagnetic field measurement.

Isotropic antenna based on Rydberg atoms.

Governed by the hairy ball theorem, classical antennas with isotropic responses to linearly polarized radio waves are unrealizable. Also, their calibrations face a causal dilemma. Therefore, radio wave measurements based on classical antennas are challenging to achieve high accuracy. This work shows that the antenna based on Rydberg atoms can theoretically achieve an ideal isotropic response to linearly polarized radio waves; that is, it has zero isotropic deviation. Although this conclusion is straightforward, it is not theoretically clear when complex atomic energy levels are taken into account. Experimental results of isotropic deviation within 5 dB and 0.3 dB possible with optimization in microwave and terahertz wave measurements support the theory and is at least 15 dB improvement than the classical omnidirectional antenna. Combined with the SI traceable and ultrawideband property, the ideal isotropic response will make radio wave measurement based on atomic antenna much more accurate and reliable than the traditional method. This isotropic atomic antenna is an excellent example of what a tailored quantum sensor can realize, but a classical sensor cannot. It has crucial applications in fields such as radio wave electrometry.

Three-dimensional quantum imaging of dynamic targets using quantum compressed sensing.

Quantum imaging based on entangled light sources exhibits enhanced background resistance compared to conventional imaging techniques in low-light conditions. However, direct imaging of dynamic targets remains challenging due to the limited count rate of entangled photons. In this paper, we propose a quantum imaging method based on quantum compressed sensing that leverages the strong correlation characteristics of entangled photons and the randomness inherent in photon pair generation and detection. This approach enables the construction of a compressed sensing system capable of directly imaging high-speed dynamic targets. The results demonstrate that our system successfully achieves imaging of a target rotating at a frequency of 10 kHz, while maintaining an impressive data compression rate of 10-6. This proposed method introduces a pioneering approach for the practical implementation of quantum imaging in real-world scenarios.

Anomalous layer-dependent photoluminescence spectra of supertwisted spiral WS2.

Twisted stacking of two-dimensional materials with broken inversion symmetry, such as spiral MoTe2 nanopyramids and supertwisted spiral WS2, emerge extremely strong second- and third-harmonic generation. Unlike well-studied nonlinear optical effects in these newly synthesized layered materials, photoluminescence (PL) spectra and exciton information involving their optoelectronic applications remain unknown. Here, we report layer- and power-dependent PL spectra of the supertwisted spiral WS2. The anomalous layer-dependent PL evolutions that PL intensity almost linearly increases with the rise of layer thickness have been determined. Furthermore, from the power-dependent spectra, we find the power exponents of the supertwisted spiral WS2 are smaller than 1, while those of the conventional multilayer WS2 are bigger than 1. These two abnormal phenomena indicate the enlarged interlayer spacing and the decoupling interlayer interaction in the supertwisted spiral WS2. These observations provide insight into PL features in the supertwisted spiral materials and may pave the way for further optoelectronic devices based on the twisted stacking materials.

Radio frequency electric field-enhanced sensing based on the Rydberg atom-based superheterodyne receiver.

We present enhanced sensing of a radio frequency (RF) electric field (E-field) by the combined polarizability of Rydberg atoms and the optimized local oscillator (LO) field of a superheterodyne receiver. Our modified theoretical model reveals the dependencies of the sensitivity of E-field amplitude measurement on the polarizability of Rydberg states and the strength of the LO field. The enhanced sensitivities of the megahertz (MHz) E-field are demonstrated at the optimal LO field for three different Rydberg states ${\rm 43D}_{5/2}$, ${\rm 60S}_{1/2}$, and ${\rm 90S}_{1/2}$. The sensitivity of 63 MHz for the ${\rm 90S}_{1/2}$ state reaches 9.6 $\times 10^{-5}\rm \,V/m/\sqrt {Hz}$, which is approximately an order of magnitude higher than those already published. This result closely approaches the sensitivity limit of a 1 cm passive dipole antenna without using an impedance matching network. This atomic sensor based on the Rydberg Stark effect with heterodyne technique is expected to boost an alternative solution to electric dipole antennas.

Optical feedback noise-immune cavity-enhanced optical heterodyne molecular spectrometry for sub-Doppler-broadened detection of C2H2: publisher's note.

This publisher's note contains a correction to Opt. Lett.49, 202 (2024)10.1364/OL.507004.

Optical feedback noise-immune cavity-enhanced optical heterodyne molecular spectrometry for sub-Doppler-broadened detection of C2H2.

A novel, to the best of our knowledge, noise-immune cavity-enhanced optical heterodyne molecular spectrometry (NICE-OHMS) has been developed, utilizing optical feedback for laser-to-cavity locking with a common distributed-feedback diode laser. The system incorporates active control of the feedback phase and feedforward control of the laser current, allowing for consecutive laser frequency detuning by scanning a piezoelectric transducer (PZT) attached to the cavity. To enhance the fidelity of the spectroscopic signal, wavelength-modulated (wm) NICE-OHMS is implemented. Benefiting from the optical feedback, a modulation frequency of 15 kHz is achieved, surpassing the frequencies typically used in traditional NICE-OHMS setups. Then, the sub-Doppler-broadened wm-NICE-OHMS signal of acetylene at 1.53 µm is observed. A seven-fold improvement in signal to noise ratio has been demonstrated compared to NICE-OHMS alone and a limit of detection of 6.1 × 10-10cm-1 is achieved.

Dynamical Detection of Topological Spectral Density.

Local density of states (LDOS) is emerging as powerful means of exploring classical-wave topological phases. However, the current LDOS detection method remains rare and merely works for static situations. Here, we introduce a generic dynamical method to detect both the static and Floquet LDOS, based on an elegant connection between dynamics of chiral density and local spectral densities. Moreover, we find that the Floquet LDOS allows to measure out Floquet quasienergy spectra and identify topological π modes. As an example, we demonstrate that both the static and Floquet higher-order topological phase can be universally identified via LDOS detection, regardless of whether the topological corner modes are in energy gaps, bands, or continuous energy spectra without band gaps. Our study opens a new avenue utilizing dynamics to detect topological spectral densities and provides a universal approach of identifying static and Floquet topological phases.

Exceptional Nexus in Bose-Einstein Condensates with Collective Dissipation.

In multistate non-Hermitian systems, higher-order exceptional points and exotic phenomena with no analogues in two-level systems arise. A paradigm is the exceptional nexus (EX), a third-order EP as the cusp singularity of exceptional arcs (EAs), that has a hybrid topological nature. Using atomic Bose-Einstein condensates to implement a dissipative three-state system, we experimentally realize an EX within a two-parameter space, despite the absence of symmetry. The engineered dissipation exhibits density dependence due to the collective atomic response to resonant light. Based on extensive analysis of the system's decay dynamics, we demonstrate the formation of an EX from the coalescence of two EAs with distinct geometries. These structures arise from the different roles played by dissipation in the strong coupling limit and quantum Zeno regime. Our Letter paves the way for exploring higher-order exceptional physics in the many-body setting of ultracold atoms.

Size-dependent photoluminescence blinking mechanisms and volume scaling of biexciton Auger recombination in single CsPbI3 perovskite quantum dots.

Determining the correlation between the size of a single quantum dot (QD) and its photoluminescence (PL) properties is a challenging task. In the study, we determine the size of each QD by measuring its absorption cross section, which allows for accurate investigation of size-dependent PL blinking mechanisms and volume scaling of the biexciton Auger recombination at the single-particle level. A significant correlation between the blinking mechanism and QD size is observed under low excitation conditions. When the QD size is smaller than their Bohr diameter, single CsPbI3 perovskite QDs tend to exhibit BC-blinking, whereas they tend to exhibit Auger-blinking when the QD size exceeds their Bohr diameter. In addition, by extracting bright-state photons from the PL intensity trajectories, the effects of QD charging and surface defects on the biexcitons are effectively reduced. This allows for a more accurate measurement of the volume scaling of biexciton Auger recombination in weakly confined CsPbI3 perovskite QDs at the single-dot level, revealing a superlinear volume scaling (τXX,Auger ∝ σ1.96).

Narrow laser linewidth measurement with the optimal demodulated Lorentzian spectrum: erratum.

This erratum corrects errors in Fig. 4(b) of the original paper, Appl. Opt.63, 1847 (2023)APOPAI0003-693510.1364/AO.510265. This correction does not affect any of the results or conclusions of the aforementioned paper.

Narrow laser linewidth measurement with the optimal demodulated Lorentzian spectrum.

A method called the optimal demodulated Lorentzian spectrum is employed to precisely quantify the narrowness of a laser's linewidth. This technique relies on the coherent envelope demodulation of a spectrum obtained through short delayed self-heterodyne interferometry. Specifically, we exploit the periodic features within the coherence envelope spectrum to ascertain the delay time of the optical fiber. Furthermore, the disparity in contrast within the coherence envelope spectrum serves as a basis for estimating the laser's linewidth. By creating a plot of the coefficient of determination for the demodulated Lorentzian spectrum fitting in relation to the estimated linewidth values, we identify the existence of an optimal Lorentzian spectrum. The corresponding laser linewidth found closest to the true value is deemed optimal. This method holds particular significance for accurately measuring the linewidth of lasers characterized as narrow or ultranarrow.

Quantum sensing of microwave electric fields based on Rydberg atoms.

Microwave electric field (MW E-field) sensing is important for a wide range of applications in the areas of remote sensing, radar astronomy and communications. Over the past decade, Rydberg atoms have been used in ultrasensitive, wide broadband, traceable, stealthy MW E-field sensing because of their exaggerated response to MW E-fields, plentiful optional energy levels and integratable preparation methods. This review first introduces the basic concepts of quantum sensing, the properties of Rydberg atoms and the principles of quantum sensing of MW E-fields with Rydberg atoms. An overview of this very active research direction is gradually expanding, covering the progress of sensitivity and bandwidth in Rydberg atom-based microwave sensing, superheterodyne quantum sensing with microwave-dressed Rydberg atoms, quantum-enhanced sensing of MW E-field and recent advanced quantum measurement systems and approaches to further improve the performance of MW E-field sensing. Finally, a brief outlook on future development directions is provided.

Noninvasive Skin Respiration (CO2) Measurement Based on Quartz-Enhanced Photoacoustic Spectroscopy.

A noninvasive method for disease diagnosis that does not require complex specialized laboratory facilities and chemical reagents is particularly attractive in the current medical environment. Here, we develop a noninvasive skin respiration sensor based on quartz-enhanced photoacoustic spectroscopy (QEPAS) that can monitor the skin elimination rate of carbon dioxide (CO2). A 3.8 mW distributed feedback laser emitting at 2.0 µm is used as an excitation source, and a three-dimensional (3D)-printed acoustic detection module is designed to apply to the skin as a sensor head. The performance of the noninvasive skin respiration sensor is assessed in terms of detection sensitivity, linearity, long-term stability, and water effect. A minimum detection limit of 35 ppb is achieved at the optimal integration time of 670 s. The skin respiration measurements from eight healthy volunteers are recorded, and the real-time results are analyzed.

Robust Ramsey interferometer based on a single Rydberg polariton.

We demonstrate a robust single-photon Ramsey interferometer based on a single Rydberg excitation, where the photon is stored as a Rydberg polariton in an ensemble of atoms. This coherent conversion of the photon to Rydberg polariton enables to split an incoming photon into a superposition state of two Rydberg states by applying microwave fields, which constructs two paths of interferometer. Ramsey interference fringes are demonstrated when we scan either the detuning of the microwave or the free evolution time, from which we can obtain the resonant transition frequency of two Rydberg states. We use the Ramsey-like sequence to demonstrate coherent manipulation of the stored single-photon to construct different interference patterns. In addition, the robustness of the Ramsey interferometer to the fluctuation of incoming photon numbers and optical depth (OD) of the atomic ensemble is tested, showing that the coherent of Ramsey interferometer is preserved for input photon number in a range of Rin < 15 and for OD varying from 1.0 to 4.0. The robust interferometer will find its applications in quantum precision measurement.

Identification of orbital angular momentum using atom-based spatial self-phase modulation.

Optical vortex orbital angular momentum modes, namely the twists number of the light does in one wavelength, play a critical role in quantum-information coding, super-resolution imaging, and high-precision optical measurement. Here, we present the identification of the orbital angular momentum modes based on spatial self-phase modulation in rubidium atomic vapor. The refractive index of atomic medium is spatially modulated by the focused vortex laser beam, and the resulted nonlinear phase shift of beam directly related to the orbital angular momentum modes. The output diffraction pattern carries clearly distinguishable tails, whose number and rotation direction correspond to the magnitude and sign of the input beam orbital angular momentum, respectively. Furthermore, the visualization degree of orbital angular momentums identification is adjusted on-demand in the terms of incident power and frequency detuning. These results show that the spatial self-phase modulation of atomic vapor can provide a feasible and effective way to rapidly readout the orbital angular momentum modes of vortex beam.

Geometric pattern evolution of photonic graphene in coherent atomic medium.

The photonic graphene in atoms not only has the typical photonic band structures but also exhibits controllable optical properties that are difficult to achieve in the natural graphene. Here, the evolution process of discrete diffraction patterns of a photonic graphene, which is constructed through a three-beam interference, is demonstrated experimentally in a 5S1/2 - 5P3/2 - 5D5/2 85Rb atomic vapor. The input probe beam experiences a periodic refractive index modulation when traveling through the atomic vapor, and the evolution of output patterns with honeycomb, hybrid-hexagonal, and hexagonal geometric profiles is obtained by controlling the experimental parameters of two-photon detuning and the power of the coupling field. Moreover, the Talbot images of such three kinds of periodic structure patterns at different propagating planes are observed experimentally. This work provides an ideal platform to investigate manipulation the propagation of light in artificial photonic lattices with tunable periodically varying refractive index.

Dephasing of ultracold cesium 80D5/2-Rydberg electromagnetically induced transparency.

We study Rydberg electromagnetically induced transparency (EIT) of a cascade three-level atom involving 80D5/2 state in a strong interaction regime employing a cesium ultracold cloud. In our experiment, a strong coupling laser couples 6P3/2 to 80D5/2 transition, while a weak probe, driving 6S1/2 to 6P3/2 transition, probes the coupling induced EIT signal. At the two-photon resonance, we observe that the EIT transmission decreases slowly with time, which is a signature of interaction induced metastability. The dephasing rate γOD is extracted with optical depth OD = γODt. We find that the optical depth linearly increases with time at onset for a fixed probe incident photon number Rin before saturation. The dephasing rate shows a nonlinear dependence on Rin. The dephasing mechanism is mainly attributed to the strong dipole-dipole interactions, which leads to state transfer from nD5/2 to other Rydberg states. We demonstrate that the typical transfer time τ0(80D) obtained by the state selective field ionization technique is comparable with the decay time of EIT transmission τ0(EIT). The presented experiment provides a useful tool for investigating the strong nonlinear optical effects and metastable state in Rydberg many-body systems.