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We present a compact setup for spin-, time-, and angle-resolved photoemission spectroscopy. A 10 kHz titanium sapphire laser system delivers pulses of 20 fs duration, which drive a high harmonic generation-based source for ultraviolet photons at 21 eV for photoemission. The same laser also excites the sample for pump–probe experiments. Emitted electrons pass through a hemispherical energy analyzer and a spin-filtering element. The latter is based on spin-polarized low-energy electron diffraction on an Au-passivated iridium crystal. The performance of the measurement system is discussed in terms of the resolution and efficiency of the spin filter, which are higher than those for Mott-based techniques. [ABSTRACT FROM AUTHOR]

An on-demand source of bright entangled photon pairs is desirable for quantum key distribution (QKD) and quantum repeaters. The leading candidate to generate such pairs is based on spontaneous parametric down-conversion (SPDC) in non-linear crystals. However, its pair extraction efficiency is limited to 0.1% when operating at near-unity fidelity due to multiphoton emission at high brightness. Quantum dots in photonic nanostructures can in principle overcome this limit, but the devices with high entanglement fidelity (99%) have low pair extraction efficiency (0.01%). Here, we show a measured peak entanglement fidelity of 97.5% ± 0.8% and pair extraction efficiency of 0.65% from an InAsP quantum dot in an InP photonic nanowire waveguide. We show that the generated oscillating two-photon Bell state can establish a secure key for peer-to-peer QKD. Using our time-resolved QKD scheme alleviates the need to remove the quantum dot energy splitting of the intermediate exciton states in the biexciton-exciton cascade. Spontaneous parametric down-conversion, the standard technique for generating entangled photons, is limited by low pair extraction efficiencies at near-unity fidelity. The authors show quantum dots in nanowires efficiently emit an oscillating state with near-unity entanglement fidelity and propose a time-resolved quantum key distribution protocol. [ABSTRACT FROM AUTHOR]

This report highlights the combination of the MicroTime 100 upright confocal fluorescence lifetime microscope with a Single Quantum Eos Superconducting Nanowire Single-Photon Detector (SNSPD) system as a powerful tool for photophysical research and applications. We focus on an application in materials science, photoluminescence imaging, and lifetime characterization of Cu(InGa)Se2 (CIGS) devices intended for solar cells. We demonstrate improved sensitivity, signal-to-noise ratio, and time-resolution in combination with confocal spatial resolution in the near-infrared (NIR) range, specifically in the 1000–1300 nm range. The MicroTime 100–Single Quantum Eos system shows two orders of magnitude higher signal-to-noise ratio for CIGS devices' photoluminescence imaging compared to a standard NIR-photomultiplier tube (NIR-PMT) and a three-fold improvement in time resolution, which is now limited by the laser pulse width. Our results demonstrate the advantages in terms of image quality and time resolution of SNSPDs technology for imaging in materials science. [ABSTRACT FROM AUTHOR]

One of the key challenges in developing quantum networks is to generate single photons with high brightness, purity, and long temporal coherence. Semiconductor quantum dots potentially satisfy these requirements; however, due to imperfections in the surrounding material, the coherence generally degrades with increasing excitation power yielding a broader emission spectrum. Here we overcome this power-broadening regime and demonstrate an enhanced coherence at exciton saturation where the detected count rates are highest. We detect single-photon count rates of 460 000 counts per second under pulsed laser excitation while maintaining a single-photon purity greater than 99%. Importantly, the enhanced coherence is attained with quantum dots in ultraclean wurtzite InP nanowires, where the surrounding charge traps are filled by exciting above the wurtzite InP nanowire band gap. By raising the excitation intensity, the number of possible charge configurations in the quantum dot environment is reduced, resulting in a narrower emission spectrum. Via Monte Carlo simulations we explain the observed narrowing of the emission spectrum with increasing power. Cooling down the sample to 300 mK, we further enhance the single-photon coherence twofold as compared to operation at 4.5 K, resulting in a homogeneous coherence time, T2, of 1.2 ns, and two-photon interference visibility as high as 83% under strong temporal postselection (~5% without temporal postselection). [ABSTRACT FROM AUTHOR]

A major step toward fully integrated quantum optics is the deterministic incorporation of high quality single photon sources in on-chip optical circuits. We show a novel hybrid approach in which preselected III-V single quantum dots in nanowires are transferred and integrated in silicon based photonic circuits. The quantum emitters maintain their high optical quality after integration as verified by measuring a low multiphoton probability of 0.07 ± 0.07 and emission line width as narrow as 3.45 ± 0.48 GHz. Our approach allows for optimum alignment of the quantum dot light emission to the fundamental waveguide mode resulting in very high coupling efficiencies. We estimate a coupling efficiency of 24.3 ± 1.7% from the studied single-photon source to the photonic channel and further show by finite-difference time-domain simulations that for an optimized choice of material and design the efficiency can exceed 90%. [ABSTRACT FROM AUTHOR]

Abstract: Pentacene field-effect transistors were prepared on silicon nitride membranes for scanning transmission X-ray microscopy (STXM) investigations. The membranes were modified by different self-assembled monolayers (SAMs). Pentacene was deposited atop the SAM-treated membrane and the in-plane orientation of the grains were subsequently investigated by polarization dependent STXM measurements. The grain sizes were determined and compared to those obtained from atomic force microscopy (AFM) measurements. Statistical analysis of the grain orientation was correlated with the charge carrier mobility of the films, in which we observed an increase in the mobility with increasing grain size and decreasing surface roughness of the SAM. [Copyright &y& Elsevier]

Prior to the development of pulsed lasers, one assigned a single local temperature to the lattice, the electron gas, and the spins. With the availability of ultrafast laser sources, one can now drive the temperature of these reservoirs out of equilibrium. Thus, the solid shows new internal degrees of freedom characterized by individual temperatures of the electron gas Te, the lattice Tl and the spins Ts. We demonstrate an analogous behavior in the spin polarization of a ferromagnet in an ultrafast demagnetization experiment: At the Fermi energy, the polarization is reduced faster than at deeper in the valence band. Therefore, on the femtosecond time scale, the magnetization as a macroscopic quantity does not provide the full picture of the spin dynamics: The spin polarization separates into different parts similar to how the single temperature paradigm changed with the development of ultrafast lasers. [ABSTRACT FROM AUTHOR]

Two-photon microscopy (2PM) has become an important tool in biology to study the structure and function of intact tissues in vivo . However, adult mammalian tissues such as the mouse brain are highly scattering, thereby putting fundamental limits on the achievable imaging depth, which typically reside at around 600-800 μm. In principle, shifting both the excitation as well as (fluorescence) emission light to the shortwave near-infrared (SWIR, 1000-1700 nm) region promises substantially deeper imaging in 2PM, yet this shift has proven challenging in the past due to the limited availability of detectors and probes in this wavelength region. To overcome these limitations and fully capitalize on the SWIR region, in this work, we introduce a novel array of superconducting nanowire single-photon detectors (SNSPDs) and associated custom detection electronics for use in near-infrared 2PM. The SNSPD array exhibits high efficiency and dynamic range as well as low dark-count rates over a wide wavelength range. Additionally, the electronics and software permit a seamless integration into typical 2PM systems. Together with an organic fluorescent dye emitting at 1105 nm, we report imaging depth of >1.1 mm in the in vivo mouse brain, limited mostly by available labeling density and laser properties. Our work establishes a promising, and ultimately scalable, new detector technology for SWIR 2PM that facilitates deep tissue biological imaging., Competing Interests: The authors declare the following competing financial interest(s): The following authors were employed by Single Quantum B.V. and may profit financially: N.N, J.N.L.L, A. G., H.K., M.C, MAUC, A.F. The other authors declare no competing financial interests., (© 2024 The Authors. Published by American Chemical Society.)

The analysis of proteins in the gas phase benefits from detectors that exhibit high efficiency and precise spatial resolution. Although modern secondary electron multipliers already address numerous analytical requirements, additional methods are desired for macromolecules at energies lower than currently used in post-acceleration detection. Previous studies have proven the sensitivity of superconducting detectors to high-energy particles in time-of-flight mass spectrometry. Here, we demonstrate that superconducting nanowire detectors are exceptionally well suited for quadrupole mass spectrometry and exhibit an outstanding quantum yield at low-impact energies. At energies as low as 100 eV, the sensitivity of these detectors surpasses conventional ion detectors by three orders of magnitude, and they offer the possibility to discriminate molecules by their impact energy and charge. We demonstrate three developments with these compact and sensitive devices, the recording of 2D ion beam profiles, photochemistry experiments in the gas phase, and advanced cryogenic electronics to pave the way toward highly integrated detectors.

Superconducting nanowire single-photon detectors (SNSPDs) show near unity efficiency, low dark count rate, and short recovery time. Combining these characteristics with temporal control of SNSPDs broadens their applications as in active de-latching for higher dynamic range counting or temporal filtering for pump-probe spectroscopy or LiDAR. To that end, we demonstrate active gating of an SNSPD with a minimum off-to-on rise time of 2.4 ns and a total gate length of 5.0 ns. We show how the rise time depends on the inductance of the detector in combination with the control electronics. The gate window is demonstrated to be fully and freely, electrically tunable up to 500 ns at a repetition rate of 1.0 MHz, as well as ungated, free-running operation. Control electronics to generate the gating are mounted on the 2.3 K stage of a closed-cycle sorption cryostat, while the detector is operated on the cold stage at 0.8 K. We show that the efficiency and timing jitter of the detector is not altered during the on-time of the gating window. We exploit gated operation to demonstrate a method to increase in the photon counting dynamic range by a factor 11.2, as well as temporal filtering of a strong pump in an emulated pump-probe experiment.

Light scattering by biological tissues sets a limit to the penetration depth of high-resolution optical microscopy imaging of live mammals in vivo. An effective approach to reduce light scattering and increase imaging depth is to extend the excitation and emission wavelengths to the second near-infrared window (NIR-II) at >1,000 nm, also called the short-wavelength infrared window. Here we show biocompatible core-shell lead sulfide/cadmium sulfide quantum dots emitting at ~1,880 nm and superconducting nanowire single-photon detectors for single-photon detection up to 2,000 nm, enabling a one-photon excitation fluorescence imaging window in the 1,700-2,000 nm (NIR-IIc) range with 1,650 nm excitation-the longest one-photon excitation and emission for in vivo mouse imaging so far. Confocal fluorescence imaging in NIR-IIc reached an imaging depth of ~1,100 μm through an intact mouse head, and enabled non-invasive cellular-resolution imaging in the inguinal lymph nodes of mice without any surgery. We achieve in vivo molecular imaging of high endothelial venules with diameters as small as ~6.6 μm, as well as CD169 + macrophages and CD3 + T cells in the lymph nodes, opening the possibility of non-invasive intravital imaging of immune trafficking in lymph nodes at the single-cell/vessel-level longitudinally., (© 2022. The Author(s), under exclusive licence to Springer Nature Limited.)

In the past decade, superconducting nanowire single-photon detectors (SNSPDs) have gradually become an indispensable part of any demanding quantum optics experiment. Until now, most SNSPDs have been coupled to single-mode fibers. SNSPDs coupled to multimode fibers have shown promising efficiencies but have yet to achieve high time resolution. For a number of applications ranging from quantum nano-photonics to bio-optics, high efficiency and high time resolution are desired at the same time. In this paper, we demonstrate the role of polarization on the efficiency of multimode-fiber-coupled detectors and fabricated high-performance 20 µm, 25 µm, and 50 µm diameter detectors targeted for visible, near-infrared, and telecom wavelengths. A custom-built setup was used to simulate realistic experiments with randomized modes in the fiber. We achieved over 80% system efficiency and $ {\lt} {20}\;{\rm ps}$<20ps timing jitter for 20 µm SNSPDs. Also, we realized 70% system efficiency and $ {\lt} {20}\;{\rm ps}$<20ps timing jitter for 50 µm SNSPDs. The high-efficiency multimode-fiber-coupled SNSPDs with unparalleled time resolution will benefit various quantum optics experiments and applications in the future.

We analyze the degree of entanglement measurable from a quantum dot via the biexciton-exciton cascade as a function of the exciton fine-structure splitting and the detection time resolution. We show that the time-energy uncertainty relation provides means to measure a high entanglement even in presence of a finite fine-structure splitting when a detection system with high temporal resolution is employed. Still, in many applications it would be beneficial if the fine-structure splitting could be compensated to zero. To solve this problem, we propose an all-optical approach with rotating waveplates to erase this fine-structure splitting completely which should allow obtaining a high degree of entanglement with near-unity efficiency. Our optical approach is possible with current technology and is also compatible with any quantum dot showing fine-structure splitting. This bears the advantage that for example the fine-structure splitting of quantum dots in nanowires and micropillars can be directly compensated without the need for further sample processing.

The laser-driven ultrafast demagnetization effect is one of the long-standing problems in solid-state physics. The time scale is given not only by the transfer of energy, but also by the transport of angular momentum away from the spin system. Through a double-pulse experiment resembling two-dimensional spectroscopy, we separate the different pathways by their nonlinear properties. We find (a) that the loss of magnetization within 400 fs is not affected by the previous excitations (linear process), and (b) we observe a picosecond demagnetization contribution that is strongly affected by the previous excitations. Our experimental approach is useful not only for studying femtosecond spin dynamics, but can also be adapted to other problems in solid-state dynamics.

Quantum light plays a pivotal role in modern science and future photonic applications. Since the advent of integrated quantum nanophotonics different material platforms based on III-V nanostructures-, colour centers-, and nonlinear waveguides as on-chip light sources have been investigated. Each platform has unique advantages and limitations; however, all implementations face major challenges with filtering of individual quantum states, scalable integration, deterministic multiplexing of selected quantum emitters, and on-chip excitation suppression. Here we overcome all of these challenges with a hybrid and scalable approach, where single III-V quantum emitters are positioned and deterministically integrated in a complementary metal-oxide-semiconductor-compatible photonic circuit. We demonstrate reconfigurable on-chip single-photon filtering and wavelength division multiplexing with a foot print one million times smaller than similar table-top approaches, while offering excitation suppression of more than 95 dB and efficient routing of single photons over a bandwidth of 40 nm. Our work marks an important step to harvest quantum optical technologies' full potential.Combining different integration platforms on the same chip is currently one of the main challenges for quantum technologies. Here, Elshaari et al. show III-V Quantum Dots embedded in nanowires operating in a CMOS compatible circuit, with controlled on-chip filtering and tunable routing.

The ultrafast demagnetization process allows for the generation of femtosecond spin current pulses. Here, we present a thermodynamic model of the spin current generation process, based on the chemical potential gradients as the driving force for the spin current. We demonstrate that the laser-induced spin current can be estimated by an easy to understand diffusion model.

We present the first single-shot images of ferromagnetic, nanoscale spin order taken with femtosecond x-ray pulses. X-ray-induced electron and spin dynamics can be outrun with pulses shorter than 80 fs in the investigated fluence regime, and no permanent aftereffects in the samples are observed below a fluence of 25 mJ/cm(2). Employing resonant spatially muliplexed x-ray holography results in a low imaging threshold of 5 mJ/cm(2). Our results open new ways to combine ultrafast laser spectroscopy with sequential snapshot imaging on a single sample, generating a movie of excited state dynamics.