Single-photon Frequency Upconversion Research Articles

Mid-infrared single-photon upconversion spectroscopy enabled by nonlocal wavelength-to-time mapping.

Ultrasensitive spectroscopy is an essential component in mid-infrared (MIR) technology. However, the drawbacks of MIR detectors pose challenges to robust MIR spectroscopy at the single-photon level. We propose an MIR single-photon frequency upconversion spectroscopy nonlocally mapping the MIR information to the time domain. Broadband MIR photons from spontaneous parametric downconversion are frequency-upconverted to the near-infrared band with quantum correlation preservation. Via the group delay of fiber, the MIR spectral information within a 1.18-micrometer bandwidth of 2.76 to 3.94 micrometers is then successfully projected to arrival times of correlated photon pairs. Under the conditions of 6.4 × 106 photons per second illumination, the transmission spectra of polymers with single-photon sensitivity are demonstrated using single-pixel detectors. The developed approach circumvents scanning and frequency selection instability, which stands out for its inherent compatibility for evolving environments and scalability for various wavelengths. Because of its high sensitivity and robustness, characterization of biochemical samples and weak measurement of quantum systems are possible to foresee.

Hot-band absorption assisted single-photon frequency upconversion luminescent nanophotosensitizer for 808 nm light triggered photodynamic immunotherapy of cancer.

Frequency upconversion luminescence (FUCL) based on hot-band absorption has attracted considerable attention in bioimaging and phototherapy fields for deep-seated cancer treatment. Photoimmunotherapy, a promising therapeutic approach induced by photodynamic therapy (PDT), can selectively kill cancer cells, reverse the immunosuppressive system, boost host immune response, and elicit durable antitumor immunity. To date, few near-infrared organic photosensitizers for photodynamic immunotherapy have been reported based on hot-band absorption. Herein, we report an upconversion luminescent phthalocyanine photosensitizer PdPc(OBu)8 with anti-Stokes emission at 748 nm and highly efficient singlet oxygen generation with hot-band absorption at 808 nm. Taking advantage of nanoliposomes, FUCL phthalocyanine nano-photosensitizers (PdPc NPs) were obtained to reduce the aggregation-caused quenching and improve water solubility and biocompatibility. PdPc NPs could be effectively accumulated in tumor tissues through intravenous administration, causing FUCL-induced PDT under 808 nm irradiation. Considering its finite immune responses and tumor ablation after PDT, a combination of PdPc NP-based PDT with checkpoint inhibitors (anti-PD-L1) for near-infrared photoimmunotherapy has been used to potentiate the antitumor efficacy that could simultaneously ablate primary tumors and inhibit the progression of distant tumors. This study can promote the development of upconversion-based PDT combined with immunotherapy for tumor precision therapy.

Mid-infrared single-photon upconversion spectroscopy based on temporal-spectral quantum correlation

Promoting the sensitivity of mid-infrared (MIR) spectroscopy to the single-photon level is a critical need for investigating photosensitive biological samples and chemical reactions. MIR spectroscopy based on frequency upconversion is a compelling pioneer allowing high-efficiency MIR spectral measurement with well-developed single-photon detectors, which overcomes the main limitations of high thermal noise of current MIR detectors. However, noise from other nonlinear processes caused by strong pump fields hinders the development of the upconversion-based MIR spectroscopy to reach the single-photon level. Here, a broadband MIR single-photon frequency upconversion spectroscopy is demonstrated based on the temporal-spectral quantum correlation of non-degenerate photon pairs, which is well preserved in the frequency upconversion process and is fully used in extracting the signals from tremendous noise caused by the strong pump. A correlation spectrum broader than 660 nm is achieved and applied for the demonstration of sample identification under a low incident photon flux of 0.09 average photons per pulse. The system is featured with non-destructive and robust operation, which makes single-photon-level MIR spectroscopy an appealing option in biochemical applications.

High-Efficiency Broadband Near-Infrared Single-Photon Frequency Upconversion and Detection**Supported by the National Natural Science Foundation of China under Grant Nos. 11722431, 11674099 and 11621404, and the Program of Introducing Talents of Discipline to Universities under Grant No. B12024.

We propose and demonstrate a high efficiency broadband near infrared single-photon upconversion and detection with a broadband pump laser based on sum frequency conversion in the PPLN crystal. By using a pump laser centered at 1040 nm with a spectral bandwidth of 10 nm, the signal single-photons centered at 1562 nm with a broadband bandwidth up to 7.2 nm are frequency-converted from the near infrared to the visible regime. A maximum conversion efficiency of 18.8% is achieved, while the background noise is measured to be only 1.2 × 10−3 counts/pulse. The corresponding spectral linewidth of the upconverted photons is 0.2 nm. This scheme of broadband infrared single-photon upconversion and detection provides potential solutions in infrared laser ranging, broadband infrared imaging and quantum key distribution.

Excited-state lifetime measurement of silicon vacancy centers in diamond by single-photon frequency upconversion

We report a method with high time resolution to measure the excited-state lifetime of silicon vacancy centers in bulk diamond avoiding timing jitter from the single-photon detectors. Frequency upconversion of the fluorescence emitted from silicon vacancy centers was achieved from 738 nm to 436 nm via sum frequency generation with a short pump pulse. The excited-state lifetime can be obtained by measuring the intensity of upconverted light while the pump delay changes. As a probe, a pump laser with pulse duration of 11 ps provided a high temporal resolution of the measurement. The lifetime extracted from the pump–probe curve was 0.755 ns, which was comparable to the timing jitter of the single-photon detectors.

Luminescent Probes for Sensitive Detection of pH Changes in Live Cells through Two Near-Infrared Luminescence Channels.

Two water-soluble near-infrared luminescent probes, which possess both conventional intense Stokes fluorescence and unique single-photon frequency upconversion luminescence (FUCL), were developed for sensitive and selective detection of pH changes in live cells. The water solubility and biocompatibility of these probes were achieved by introducing mannose residues through 2,2'-(ethylenedioxy)diethylamine tethered spacers to a near-infrared conventional fluorescence (CF) and FUCL organic fluorophore. At a pH higher than 7.4, the probes have ring-closed spirocyclic lactam structures, thus are colorless and nonfluorescent. Nevertheless, they sensitively respond to acidic pH values, with a drastic structural change to ring-opened spirocyclic lactam forms, which cause significant absorbance increases at 714 nm. Correspondingly, their near-infrared CF and FUCL intensities at 740 nm are also significantly enhanced when excited by 690 and 808 nm, respectively. The probes hold a variety of advantages such as high sensitivity, excellent reversibility and selectivity to pH over metal ions, low cellular autofluorescence background interference, good cell membrane permeability and photostability, as well as low cytotoxicity. Our results have successfully proven that these probes can visualize intracellular lysosomal pH changes in live cells by monitoring both near-infrared CF and FUCL changes.

Efficiency enhancement for the orbital angular momentum photon quantum interface via single photon frequency upconversion

As the application of orbital angular momentum (OAM) of photon quantum in quantum communication, the OAM photon quantum interface for the transmission wavelength from the telecom communication quantum information storage in visible regime is required. Here we demonstrate the efficiency enhancement for the OAM photon quantum interface based on the frequency upconversion from telecom wavelength to visible regime by sum-frequency generation. The infrared photons at 1 558 nm carrying different OAM values could be converted to the visible regime at 622.2 nm with the optimal efficiency via adjusting the pump beam waist radius and intensity.

Quantum detector tomography of a single-photon frequency upconversion detection system.

We experimentally presented a full quantum detector tomography of a synchronously pumped infrared single-photon frequency upconversion detector. A maximum detection efficiency of 37.6% was achieved at the telecom wavelength of 1558 nm with a background noise about 1.0 × 10-3 counts/pulse. The corresponding internal quantum conversion efficiency reached as high as 84.4%. The detector was then systematically characterized at different pump powers to investigate the quantum decoherence behavior. Here the reconstructed positive operator valued measure elements were equivalently illustrated with the Wigner function formalism, where the quantum feature of the detector is manifested by the presence of negative values of the Wigner function. In our experiment, pronounced negativities were attained due to the high detection efficiency and low background noise, explicitly showing the quantum feature of the detector. Such quantum detector could be useful in optical quantum state engineering, quantum information processing and communication.

Spatial modulation characteristics of single-photon frequency up-conversion systems pumped by Gaussian laser beam

In a Gaussian laser beam pumped single-photon frequency up-conversion system, the spatial distribution of the conversion efficiency is calculated, which strongly depends on the intensity distribution of the pump beam and leads to a spatial modulation of the output single photons. As a result, by simply varying the Gaussian pump beam intensity and the beam size, the converted photons could be modulated spatially and exhibit a programmable distribution. This will be meaningful for the researches on quantum communication and quantum manipulation based on frequency up-conversion system.

Two-dimensional infrared and mid-infrared imaging by single-photon frequency upconversion

Single-photon frequency upconversion is an effective method of infrared single-photon detection and imaging by converting the long-wavelength photons to shorter wavelengths to match the detector’s spectral response. We realized few-photon level 2D infrared imaging with a coincidence frequency upconversion system in a bulk periodically poled lithium niobate crystal. Moreover, the infrared photons carrying orbital angular momentum were converted to the visible regime with high efficiency, while the orbital angular momentum of the photons was well conserved during the frequency upconversion process. The single-photon frequency upconversion method was also used for mid-infrared imaging at 3.39 µm with high efficiency and low noise.

Efficient mid-infrared single-photon frequency upconversion detection with ultra-low background counts

We demonstrate an efficient mid-infrared single-photon detection system with ultra-low background counts based on the frequency upconversion detection technique. The signal photons of 3.39 μm came from a He–Ne laser and the pump beam was provided by a mode-locked ytterbium-doped fiber laser. Taking into account the pulsed pumping and continuous-wave signaling scheme, the peak conversion efficiency of 64% was achieved at an average pump power of 28.3 mW. The corresponding detection efficiency was inferred to be 6.1% with ultra-low background counts of 400 s−1.

Synchronized Fiber Lasers for Efficient Coincidence Single-Photon Frequency Upconversion

We experimentally demonstrate a compact synchronized fiber laser system that enables fast and efficient coincidence single-photon frequency upconversion detection. Robust synchronization between the pump and signal pulses was achieved with a long-term stability. Moreover, the synchronized pulses were wellmatching in both of the time and spectrum domains. As a result, a coincidence single-photon frequency upconversion was realized with a conversion efficiency of 91.8% and low background counts around 2.8 × 103 s-1.

Photon correlation in single-photon frequency upconversion

We experimentally investigated the intensity cross-correlation between the upconverted photons and the unconverted photons in the single-photon frequency upconversion process with multi-longitudinal mode pump and signal sources. In theoretical analysis, with this multi-longitudinal mode of both signal and pump sources system, the properties of the signal photons could also be maintained as in the single-mode frequency upconversion system. Experimentally, based on the conversion efficiency of 80.5%, the joint probability of simultaneously detecting at upconverted and unconverted photons showed an anti-correlation as a function of conversion efficiency which indicated the upconverted photons were one-to-one from the signal photons. While due to the coherent state of the signal photons, the intensity cross-correlation function g(2)(0) was shown to be equal to unity at any conversion efficiency, agreeing with the theoretical prediction. This study will benefit the high-speed wavelength-tunable quantum state translation or photonic quantum interface together with the mature frequency tuning or longitudinal mode selection techniques.

Photon-counting 155 μm optical communications with pulse-position modulation and a multimode upconversion single-photon receiver

We report single-photon frequency upconversion of multimode light from 1.55 to 0.532microm and demonstrate an end-to-end optical link that emulates photon-starved communications and atmospheric propagation. Using 64-ary pulse-position modulation and a half-rate serially concatenated turbo code we achieve a decoded efficiency of 0.3 detected photons/bit.

Temporal and spectral control of single-photon frequency upconversion for pulsed radiation

We demonstrate efficient single-photon detection at 1.04 μm with quite low background counts by using the frequency upconversion detection technique with pulsed single-photon source and strong pump field prepared from two synchronized fiber lasers. Temporal and spectral control of the pump and signal lasers enabled an upconversion efficiency of 81.1%. As the system was pumped at a wavelength longer than that of the signal, the corresponding background counts were reduced down to 1.5×103 s−1 due to efficient suppression of parametric fluorescence in the periodic poled lithium niobate crystal.

Erasing Distinguishability Using Quantum Frequency Up-Conversion

The frequency distinguishability of two single photons was successfully erased using single photon frequency up-conversion. A frequency nondegenerate photon pair generated via spontaneous four-wave mixing in a dispersion shifted fiber was used to emulate two telecom-band single photons that were in the same temporal mode but in different frequency modes. The frequencies of these photons were converted to the same frequency by using the sum-frequency generation process in periodically poled lithium niobate waveguides, while maintaining their temporal indistinguishability. As a result, the two converted photons exhibited a nonclassical dip in a Hong-Ou-Mandel quantum interference experiment. The present scheme will add flexibility to networking quantum information systems that use photons with various wavelengths.

Efficient single-photon frequency upconversion at 1.06 μm with ultralow background counts

We demonstrated an efficient single-photon frequency upconversion system for the infrared photons at 1.06 μm with ultralow background counts. By pumping the system at a longer wavelength than that of the single-photon signal, the background counts caused by the pump-induced parametric fluorescence in the nonlinear crystal were reduced markedly. We achieved so far the lowest noise of ∼150/s for a near unity conversion efficiency.

Single-photon frequency up-conversion with multimode pumping

Efficient single-photon frequency up-conversion was demonstrated under strong multi-longitudinal-mode pump, where the incident single-photon state was converted to a superposition state after the nonlinear interaction with the multimode pump field. Through frequency summing with a sufficiently strong multimode pump at $1.06\text{ }\ensuremath{\mu}\text{m}$, a single-photon signal at $1.55\text{ }\ensuremath{\mu}\text{m}$ was up-converted to the visible replicas near $0.63\text{ }\ensuremath{\mu}\text{m}$ with a nearly unity efficiency. This may support tunable multimode photonic quantum-information interface and precise wavelength control on single-photon manipulation.

Efficient and stable single-photon counting at 155 μm by intracavity frequency upconversion

A single-photon signal at 1.55 microm was converted to the visible region by sum-frequency mixing with a strong pumping beam at 1064 nm in a periodically poled lithium niobate crystal placed in a diode-pumped Nd:YVO4 laser cavity. As the intracavity pump laser could be automatically stabilized without cavity lock, robust long-term stability was demonstrated for single-photon frequency upconversion, with a conversion efficiency of 74.3%. Such a stable single-photon upconversion was demonstrated to be efficient and robust for single-photon counting at 1550 nm, and the corresponding background noise was measured at less than 420 x 10(3) s(-1).