Single-photon Process Research Articles

Off-Normal Polarized Single-Photon Emission with Anisotropic Holography Metasurfaces.

Solid-state quantum emitters (QEs) with arbitrary direction emission and well-defined polarization are critical for scalable single-photon sources and quantum information processing. However, the design strategy for on-chip generation of off-normal photon emission with high-purity polarization characteristics has so far remained elusive. Here, we introduce the anisotropic holography metasurfaces for efficiently manipulating the emission direction and polarization of QE. The proposed method offers a flexible way to realize phase matching in surface plasmon scattering with spatially varying filling factors and provides an efficient route for designing advanced QE-coupled metasurfaces. By nonradiatively coupling nanodiamonds with metasurfaces, we experimentally demonstrate on-chip generation of well-collimated single-photon emission propagating along off-normal directions (i.e., 20° and 30°) featuring a divergence angle lower than 2.5°. The experimental average degree of linear polarization attains up to >0.98, thereby revealing markedly high polarization purity. This study facilitates applications of QEs in the deployment of integrated quantum networks.

Photodissociation spectra of single trapped CaOH+ molecular ions.

Molecular ions that are generated by chemical reactions with trapped atomic ions can serve as an accessible testbed for developing molecular quantum technologies. On the other hand, they are also a hindrance to scaling up quantum computers based on atomic ions, as unavoidable reactions with background gases destroy the information carriers. Here, we investigate the single- and two-photon dissociation processes of single CaOH+ molecular ions co-trapped in Ca+ ion crystals using a femtosecond laser system. We report the photodissociation cross section spectra of CaOH+ for single-photon processes at λ = 245-275 nm and for two-photon processes at λ = 500-540 nm. Measurements are interpreted with quantum-chemical calculations, which predict the photodissociation threshold for CaOH+ → Ca+ + OH at 265nm. This result can serve as a basis for dissociation-based spectroscopy for studying the internal structure of CaOH+. The result also gives a prescription for recycling Ca+ ions in large-scale trapped Ca+ quantum experiments from undesired CaOH+ ions formed in the presence of background water vapor.

Cryogenic Photoelectron Spectroscopic and Theoretical Study of the Electronic and Geometric Structures of Undercoordinated Osmium Chloride Anions OsCln- (n = 3-5).

A series of anionic transition metal halides, OsCln- (n = 3-5), have been investigated using a newly developed, home-constructed, cryogenic anion cluster photoelectron spectroscopy. The target anionic species are generated through collision-induced dissociation in a two-stage ion funnel. The measured vertical detachment energies (VDEs) are 3.48, 4.54, and 4.81 eV for n = 3, 4, and 5, respectively. Density functional theory calculations at the B3LYP-D3(BJ)//aug-cc-pVTZ(-pp) level predict the lowest energy structures of the atomic form of OsCln- (n = 3-5) to be a quintet triangle, quartet square, and quintet square-based pyramid, respectively. The CCSD(T)-calculated VDEs and corresponding adiabatic detachment energies agree well with our experimental measurements. Analysis of the corresponding frontier molecular orbitals and charge density differences suggests that the d-orbitals of the transition metal Os play a primary role in the single-photon detachment processes, and the detached electrons originating from different molecular orbitals are distinguishable.

Near-infrared light-triggered prodrug photolysis by one-step energy transfer

Prodrug photolysis enables spatiotemporal control of drug release at the desired lesions. For photoactivated therapy, near-infrared (NIR) light is preferable due to its deep tissue penetration and low phototoxicity. However, most of the photocleavable groups cannot be directly activated by NIR light. Here, we report a upconversion-like process via only one step of energy transfer for NIR light-triggered prodrug photolysis. We utilize a photosensitizer (PS) that can be activated via singlet-triplet (S-T) absorption and achieve photolysis of boron-dipyrromethene (BODIPY)-based prodrugs via triplet-triplet energy transfer. Using the strategy, NIR light can achieve green light-responsive photolysis with a single-photon process. A wide range of drugs and bioactive molecules are designed and demonstrated to be released under low-irradiance NIR light (100 mW/cm2, 5 min) with high yields (up to 87%). Moreover, a micellar nanosystem encapsulating both PS and prodrug is developed to demonstrate the practicality of our strategy in normoxia aqueous environment for cancer therapy. This study may advance the development of photocleavable prodrugs and photoresponsive drug delivery systems for photo-activated therapy.

Strong coupling dynamics of driven quantum systems with permanent dipoles

Many optically active systems possess spatially asymmetric electron orbitals. These generate permanent dipole moments, which can be stronger than the corresponding transition dipole moments, significantly affecting the system dynamics and creating polarized Fock states of light. We derive a master equation for these systems with an externally applied driving field by employing an optical polaron transformation that captures the photon mode polarization induced by the permanent dipoles. This provides an intuitive framework to explore their influence on the system dynamics and emission spectrum. We find that permanent dipoles introduce multiple-photon processes and a photon sideband, which causes substantial modifications to single-photon transition dipole processes. In the presence of an external drive, permanent dipoles lead to an additional process that we show can be exploited to control the decoherence and transition rates. We derive the emission spectrum of the system, highlighting experimentally detectable signatures of optical polarons, and measurements that can identify the parameters in the system Hamiltonian, the magnitude of the differences in the permanent dipoles, and the steady-state populations of the system.

Single- and two-photon absorption induced all-optical control of gallium selenide integrated silicon nitride photonic devices in the 700–800 nm wavelength range

In this work, we report single- and two-photon absorption (TPA) induced transmission and resonance modulation in a multilayer gallium selenide (GaSe) integrated silicon nitride (Si3N4) waveguide and ring resonator operating in the 700–800 nm wavelength range. Intensity dependent saturable absorption at low optical powers followed by TPA at higher power levels in GaSe integrated Si3N4 waveguides is observed at 785 nm pulsed laser excitation. A TPA coefficient of 0.117 cm/GW for the GaSe–Si3N4 composite waveguide and a three-photon absorption coefficient of 7.876 × 10−6 cm3/GW2 for the bare Si3N4 waveguide are extracted from intensity dependent transmission measurements. The single-photon absorption process induced by a blue laser incident on the multilayer GaSe transferred on top of the Si3N4 ring resonator is used for all-optical resonance tuning through the free-carrier refraction effect. A strong blue shift of the resonance by ∼12.3 pm/mW combined with resonance broadening is observed due to the free-carrier induced refractive index and absorption modulation. The TPA in the GaSe integrated Si3N4 ring resonator is also shown to result in a blue shift of the resonances excited using a 785 nm pulsed laser. This work demonstrates the all-optical control of 2D material integrated Si3N4 guided-wave structures operating in the shorter near-infrared wavelength range with potential applications in integrated quantum photonics, miniaturized sensing devices, and biomedical imaging.

Cutaneous Porphyrin Exhibits Anti-Stokes Fluorescence Emission Under Continuous Wave Laser Excitation

We report the discovery that anti-Stokes fluorescence emission can be induced from porphyrins by continuous wave (cw) laser excitation. An anti-Stokes spectroscopy and imaging technique with an integrated multimodal imaging system was developed to study cutaneous porphyrin in psoriasis, acne, and nasal skin. We experimentally demonstrated that under 785 nm cw laser excitation, photoporphyrin IX (PpIX) powder exhibited anti-Stokes fluorescence with its intensity linearly depending on the excitation power, confirmed that it is a single-photon process. Anti-Stokes fluorescence imaging of psoriasis scale, acne sebum smear, and nasal skin was performed. The results showed that Anti-Stokes fluorescence is sensitive and also specific for porphyrin detection without interference from other skin fluorophores.

Generation of collimated extreme ultraviolet radiation by single-photon process

Generating laser with short wavelength is a bottleneck problem in laser technology. The current applicable table-top extreme ultraviolet (EUV) lasers are all generated by multi-photon process with low efficiency. By utilizing metastable helium atoms excited by microwave and irradiated by a resonant laser, here we report the development of 58.4 nm collimated radiation by single-photon-excitation related anti-Stokes Raman scattering (ASRS). The conversion efficiency is much higher than that of high harmonic generation (HHG). The same divergence of 1.4 mrad as that of excitation laser indicates its stimulating character. Our results show an applicable path towards up-conversion by single-photon process to generate table-top EUV lasers.

Charge sharing simulations and measurements for digital algorithms aiming at subpixel resolution in photon counting pixel detectors

Hybrid pixel detectors are segmented devices used for X-ray detection that consist of a sensor attached to the readout electronics. Detectors working in single-photon counting mode process each incoming photon individually, have essentially infinite dynamic range, and by applying energy discrimination they provide noiseless imaging. To improve the resolution of the detector and allow operation with high-intensity photon fluxes, the pixel size is reduced. However, with decreasing pixel size, a charge sharing effect is more prominent. This leads to false event registration or omitting the event, and degradation of the energy resolution of the detector. Algorithms aiming at reducing the influence of charge sharing have already been implemented on-chip. However, the spatial resolution of the detector can be increased beyond the physical size of the pixel if the charge proportions collected by neighboring pixels are analyzed.The simulations show that charge cloud size referred to pixel size and noise are the key parameters that determine the accuracy of the subpixel algorithm. The article shows the concept of subpixel algorithm and the simulations for different detector parameters and approximation algorithms. The slanted-edge method was implemented to quantify the resolution of detectors consisting standard readout architecture. The chips were simulated and tested to verify the influence of different bias voltages, sensor materials, and thicknesses on charge sharing and as a consequence on the detector resolution. The simulated and measured edge spread functions were compared. The results show that the simulator can be used to describe the spatial resolution of the detectors, and can be used for further studies of the resolution of detectors with subpixel algorithm implemented.

Two-Photon Excitation of Silicon-Vacancy Centers in Nanodiamonds for All-Optical Thermometry with a Noise Floor of 6.6 mK·Hz–1/2

In this paper, we introduce ultrasensitive all-optical nanothermometry using high figure-of-merit nanodiamonds with silicon-vacancy (SiV) centers. In contrast to the commonly used single-photon process, we have adopted a two-photon approach to achieve efficient excitation of SiV centers in nanodiamonds. Based on the developed intensity-projected scheme, we have experimentally achieved a noise floor of 6.6 mK·Hz–1/2 using nanodiamonds. This serves as a new record of temperature resolution in the relevant field. Particularly, this simplified method allows us to reflect the temperature-induced spectral shift without wavelength scanning via a spectrometer. Furthermore, we demonstrate that the two-photon excitation of SiV centers has been thermally activated, as indicated by an elevated fluorescence intensity accompanied by a temperature increase. Our findings offer an opportunity for harnessing SiV-based nanothermometry in an easy-to-use manner and open the road for the development of practical applications in complicated environments such as living cells.

Nanosecond Photoemission near the Potential Barrier of a Schottky Emitter

Nanosecond electron pulses are appealing for ultrafast imaging and electron-gating applications, where tunable currents and narrow energy spreads are desirable. Here, we demonstrate photoemission from a Schottky emitter triggered by nanosecond laser pulses. Using photon energies optimally tuned to the emission potential barrier, we generate pulses containing over ${10}^{5}$ electrons with energy spreads below 1 eV by means of a prompt single-photon photoemission process. These results are consistent with a theoretical model of laser-triggered electron emission and energetic broadening during propagation and can be widely implemented.

Новые апконверсионные объемные и нанолюминофоры на основе Sr-=SUB=-2-=/SUB=-Y-=SUB=-8-x-y-=/SUB=-Yb-=SUB=-y-=/SUB=-Tm-=SUB=-x-=/SUB=-Si-=SUB=-6-=/SUB=-O-=SUB=-26-=/SUB=-

Polycrystalline phosphors with a Sr2Y8-x-yYbyTmxSi6O26 (x=0.005-0.5, y=0.2,0.3) total formula were synthesized. Nanoluminophor has been obtained from the Sr2Y7.695Yb0.3Tm0.005Si6O26 microcrystalline sample by the vacuum electron been evaporation, in the amorphous state, with the ~10.6 nm particle size. It is found, raman spectra undergoing modification by the transition from bulk- to nanosize state. Photoluminescene spectra micro- and nanophosphors are studied. Intensity of the blue emission, by the UV ligth excitation, grows in the x=0.005-0.02 region, with the x increasing. Upconversion photoluminescence (UPCL) spectra of the bulk phosphors and nanosample based on the Sr2Y7.695Yb0.3Tm0.005Si6O26 were measurd. At the pumping power around 70.8 mW, by the laser source with the λ=980 nm, thereshold population of the 3F3 level of Tm3+ ions exist. At a power higher 70.8 mW, a sharp increase of the luminescence intensityof the bulk- and nanophosphor occurs. For the 3H4->3H6 transition thereshold pumping power absent. This indicates that, pumping, during Yb->Tm energy transer, is a single photon process.

Electron-photon interactions in the conditions of dimensional conductivity restrictions in semiconductor single quantum-size particles in interelectrodic nanogap

For quantum-size particles of the InSb, PbS, HgSe, CdSe semiconductors, a model of competition of dimensional quantum restrictions and blocking with a single-electron current and Coulomb restriction, as well as heating electrons with an electric field of the light wave, is proposed. This made it possible to explain the highly multiplicity (up to two orders of order) of a change in photoconductivity observed in conditions of tunnel conductivity, and in the conditions of the confinement --- the absence of inter-zone and inter-level photoconductivity. The resonant current peaks of quantum conductivity observed on the V-I characteristics when irritating with light of any wavelength (in the interval of 0.4-1.2 μm) are reset or shifted towards smaller voltage values. The energy minimum of quanta recorded in this case is estimated as 100 meV. The results can be useful in resolving issues of application in uncooled IR detectors, including single-photon registration. Keywords: Quantum-size particle, dimensional quantification, one-electron current, single-photon process, inter-zone and intra-zone transitions, tunnel conductivity, Coulomb restriction, quantum conductivity.

Infrared photodesorption of CO from astrophysically relevant ices studied with a free-electron laser.

The infrared excitation and photodesorption of carbon monoxide (CO) and water-containing ices have been investigated using the FEL-2 free-electron laser light source at the FELIX laboratory, Radboud University, The Netherlands. CO-water mixed ices grown on a gold-coated copper substrate at 18 K were investigated. No CO photodesorption was observed, within our detection limits, following irradiation with light resonant with the C-O vibration (4.67 μm). CO photodesorption was seen as a result of irradiation with infrared light resonant with water vibrational modes at 2.9 μm and 12 μm. Changes to the structure of the water ice, which modifies the environment of the CO in the mixed ice, were also seen subsequent to irradiation at these wavelengths. No water desorption was observed at any wavelength of irradiation. Photodesorption at both wavelengths is due to a single-photon process. Photodesorption arises due to a combination of fast and slow processes of indirect resonant photodesorption (fast), and photon-induced desorption resulting from energy accumulation in the librational heat bath of the solid water (slow) and metal-substrate-mediated laser-induced thermal desorption (slow). Estimated cross-sections for the slow processes at 2.9 μm and 12 μm were found to be ∼7.5 × 10-18 cm2 and ∼4.5 × 10-19 cm2, respectively.

Is orange carotenoid protein photoactivation a single-photon process?

In all published photoactivation mechanisms of orange carotenoid protein (OCP), absorption of a single photon by the orange dark state starts a cascade of red-shifted OCP ground-state intermediates that subsequently decay within hundreds of milliseconds, resulting in the formation of the final red form OCPR, which is the biologically active form that plays a key role in cyanobacteria photoprotection. A major challenge in deducing the photoactivation mechanism is to create a uniform description explaining both single-pulse excitation experiments, involving single-photon absorption, and continuous light irradiation experiments, where the red-shifted OCP intermediate species may undergo re-excitation. We thus investigated photoactivation of Synechocystis OCP using stationary irradiation light with a biologically relevant photon flux density coupled with nanosecond laser pulse excitation. The kinetics of photoactivation upon continuous and nanosecond pulse irradiation light show that the OCPR formation quantum yield increases with photon flux density; thus, a simple single-photon model cannot describe the data recorded for OCP in vitro. The results strongly suggest a consecutive absorption of two photons involving a red intermediate with ≈100 millisecond lifetime. This intermediate is required in the photoactivation mechanism and formation of the red active form OCPR.

In-Situ Imaging of a Light-Induced Modification Process in Organo-Silica Films via Time-Domain Brillouin Scattering.

We applied time-domain Brillouin scattering (TDBS) for the characterization of porogen-based organosilicate glass (OGS) films deposited by spin-on-glass technology and cured under different conditions. Although the chemical composition and porosity measured by Fourier-transform infrared (FTIR) spectroscopy and ellipsometric porosimetry (EP) did not show significant differences between the films, remarkable differences between them were revealed by the temporal evolution of the Brillouin frequency (BF) shift of the probe light in the TDBS. The observed modification of the BF was a signature of the light-induced modification of the films in the process of the TDBS experiments. It correlated to the different amount of carbon residue in the samples, the use of ultraviolet (UV) femtosecond probe laser pulses in our optical setup, and their intensity. In fact, probe radiation with an optical wavelength of 356 nm appeared to be effective in removing carbon residue through single-photon absorption processes, while its two-photon absorption might have led to the breaking of Si-CH3 bonds in the OSG matrix. The quantum chemical calculations confirmed the latter possibility. This discovery demonstrates the possibility of local modifications of OSG films with a nanometric resolution via nonlinear optical processes, which could be important, among other applications, for the creation of active surface sites in the area-selective deposition of atomic layers.

Effects of single-photon double photoionization and direct double Auger decay on K-shell ionization kinetics of Ar atoms interacting with XFEL pulses

In studies investigating the interaction of matter with ultraintense, ultrashort x-ray free electron laser (XFEL) pulses, the evolution kinetics are generally described by directly solving a time-dependent rate equation that considers single-photon and single-electron processes. In the present study, we show the effects of single-photon double photoionization and direct double Auger decay in the K-shell ionization kinetics of XFELs interaction with argon atoms. Because a huge number of coupled transition channels are present in the K-shell ionization, we develop a Monte Carlo method to simulate the complex ionization kinetic processes and give the level population evolution of ions and charge state distribution (CSD). The K-shell-dominated ionization dynamics of Ar irradiated by XFEL pulses with photon energies of 5000, 5500 and 6500 eV are investigated and compared with available experimental observations of the CSD. The results show that the population fractions of Ar5+, Ar6+ and Ar9+ are increased by 78%, 152% and 144%, respectively, by these higher-order processes at a photon energy of 5000 eV. Including the direct double-electron processes, the predicted CSDs are in better agreement with the experiments carried out at the photon energies of 5000, 5500 and 6500 eV. It is expected that the developed theoretical formalism can be used to more accurately calibrate the beam profile and intensity of XFELs.

Multi-channel pseudo-random coding single-photon ranging and imaging

We demonstrate a multi-channel pseudo-random coding single-photon ranging system. A pseudo-random multiplexing technique is proposed, which realizes multi-channel pseudo-random ranging only by using one single-photon detector and processing circuit. Compared with the time division multiplexing technique, it will not reduce the maximum unambiguous range while increasing the number of the ranging channel. Eight-channel pseudo-random coding single-photon ranging was realized with the ranging accuracy better than 2 cm. Moreover, photon counting imaging was realized through scanning the laser beams of the eight-channel pseudo-random ranging system. There is no crosstalk between channels, which is suitable for multi-beam long-distance single-photon Lidar.

Precise measurement of attosecond dynamics of NO molecular shape resonance

Shape resonance is an important and ubiquitous phenomenon in the process of molecular scattering and photoionization. The study of the attosecond photoemission time delay in the vicinity of the shape resonance is of great significance for understanding its intrinsic origin on a nature time scale of electron motion. In this paper, an advanced attosecond coincidence interferometer consisting of a near-infrared femtosecond light source and an extreme ultraviolet attosecond pulse train is used to study the shape resonance process of the 4σ electron of nitric oxide molecules via reconstructing attosecond harmonic beating by measuring the interference of two-photon transitions (RABBIT). The energy dependent effective ionization time delay in the vicinity of the resonance energy region is reported. By comparing the relationship between the two-photon transition delay and the one-photon transition delay, it is found that the Wigner delay of the single-photon process is the main reason for the two-photon transition delay changing with energy. The effect of continuum-continuum delay is further explored. Theoretical calculations of the initial state (bound state) and final state (resonance state) electron wave function orbits of the resonance show that the shape resonance assisted time delay is dominated by the electrons trapped in the centrifugal potential barrier.

Synthesis of Tm2WO6:Er3+ upconversion phosphor for high-contrast imaging of latent-fingerprints

A series of Tm2−xWO6:xEr3+ (where x = 0.02–0.50 mol) phosphors were synthesized successfully by the solid-state reaction method. The powder X-ray diffraction patterns of the Tm2−xWO6:xEr3+ phosphors confirmed that the as-synthesized materials belonged to the monoclinic crystalline structure, which has a P2/c (13) space group. Due to a similar ionic size and valence state of the Er3+ ions, they can easily replace the Tm3+ in the Tm2WO6 crystal lattice. High-resolution X-ray photoelectron spectroscopy was used to explore the photoelectron binding energy and chemical state of all the elements. The XPS results confirmed that the W atom coordinated octahedrally to the oxygen atoms with its highest 6+ state in the Tm2WO6 material. The upconversion luminescence intensity at 657 nm [4F9/2→4I15/2 (Er3+)], when excited at 980 nm, was enhanced with higher magnitude when increasing the doping concentration from 0.02 mol to 0.20 mol of Er3+ ions. The dependence of the laser pump power with respect to the upconversion luminescence intensity depicts that the emission at 657 nm is due to a single-photon absorption process, and the possible reasons for the number of photons involved in the excitation of the emitting state, n ≤ 1 were discussed. The Commission Internationale del'Eclairage chromaticity coordinates and decay time measured for the Tm2WO6:Er3+ phosphors were investigated. Real-time latent-fingerprint detection using Tm2WO6:Er3+ upconversion phosphor without using Yb3+ ion showed an excellent marking agent for applications in forensic science and medical diagnostics.