ABSTRACT
Multiple photon addition and subtraction applied to multi-mode thermal and sub-Poissonian fields as well as twin beams are mutually compared using one experimental setup. Twin beams (TWBs) with tight spatial correlations detected by an intensified CCD camera with high spatial resolution are used to prepare the initial fields. Up to three photons are added or subtracted to arrive at the nonclassical and non-Gaussian states. Only the photon-subtracted thermal states (TSs) remain classical. In general, the experimental photon-added states exhibit greater nonclassicality and non-Gaussianity than the comparable photon-subtracted states. Once photons are added or subtracted in twin beams, both processes result in comparable properties of the obtained states owing to twin-beam photon pairing.
ABSTRACT
Correction for 'α-Fe2O3/TiO2 3D hierarchical nanostructures for enhanced photoelectrochemical water splitting' by Hyungkyu Han et al., Nanoscale, 2017, 9, 134-142, https://doi.org/10.1039/C6NR06908H.
ABSTRACT
Two-beam states obtained by partial photon-number-resolving detection in one beam of a multi-mode twin beam are experimentally investigated using an intensified CCD camera. In these states, sub-Poissonian photon-number distributions in one beam are accompanied by sub-shot-noise fluctuations in the photon-number difference of both beams. Multi-mode character of the twin beam implying the beam nearly Poissonian statistics is critical for reaching sub-Poissonian photon-number distributions, which contrasts with the use of a two-mode squeezed vacuum state. Relative intensities of both nonclassical effects as they depend on the generation conditions are investigated both theoretically and experimentally using photon-number distributions of these fields. Fano factor, noise-reduction parameter, local and global nonclassicality depths, degree of photon-number coherence, mutual entropy as a non-Gaussianity quantifier, and negative quasi-distributions of integrated intensities are used to characterize these fields. Spatial photon-pair correlations as means for improving the field properties are employed. These states are appealing for quantum metrology and imaging including the virtual-state entangled-photon spectroscopy.
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Photon-number-resolved post-selection on one beam out of a correlated system of three beams with bi-partite photon-number correlations gives rise to joint photon-number distributions with the probabilities forming checkered patterns. These patterns originate in the convolution of two constituting photon-number distributions, one endowed with correlations in photon numbers, the other exhibiting anti-correlations in photon-number fluctuations. Using three twin beams of comparable intensity whose constituting beams suitably overlap on the photocathode of a photon-number-resolving iCCD camera, we experimentally as well as theoretically analyze the properties of such states as they change with the varying ratio of the correlated and anti-correlated contributions. The experimental photocount 2D histograms of the fields post-selected by the iCCD camera that are reconstructed by the maximum-likelihood approach confirm their non-classicality though the limited detection efficiency in post-selection conceals the checkered patterns. Contrary to this, the maximum-likelihood reconstruction of the experimental 3D photocount histogram similarly as a suitable 3D Gaussian fit, that reveal the states as they would be obtained by ideal post-selection, provide the photon-number distributions with the checkered patterns. The corresponding quasi-distributions of integrated intensities are determined. Nonclassical properties of the generated states are investigated using suitable non-classicality criteria and the corresponding non-classicality depths. These states with their correlations of varying intensity are prospective for two-photon excitations of atoms and molecules as well as two-photon spectroscopy.
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Non-classicality criteria for optical fields based on the probabilities of photocount and photon-number distributions are derived. Relations among the criteria obtained by the applied methods are revealed. Redundant criteria are identified. The performance of the fundamental criteria is tested on a set of potentially sub-Poissonian fields generated by photon-number-resolved post-selection from a mesoscopic twin beam. The corresponding non-classicality depths are determined to quantitatively compare the used criteria.
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Using a sub-Poissonian optical field generated from a weak twin beam by photon-number resolving post-selection we have simultaneously observed higher-order non-classicalities in photocount moments (sub-Poissonian statistics) and probabilities (witnessed by the Klyshko inequalities). Up to the seventh-order non-classicalities in photocount moments simultaneously with up to the eleventh-order non-classicalities in photocount probabilities have been experimentally observed. Non-classicality counting parameters of different orders as experimental counterparts of the theoretical Lee non-classicality depth have been suggested to quantify and also mutually compare the robustness of these non-classicalities against the noise.
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We report the fabrication of 3D hierarchical hetero-nanostructures composed of thin α-Fe2O3 nanoflakes branched on TiO2 nanotubes. The novel α-Fe2O3/TiO2 hierarchical nanostructures, synthesized on FTO through a multi-step hydrothermal process, exhibit enhanced performances in photo-electrochemical water splitting and in the photocatalytic degradation of an organic dye, with respect to pure TiO2 nanotubes. An enhanced separation of photogenerated charge carriers is here proposed as the main factor for the observed photo-activities: electrons photogenerated in TiO2 are efficiently collected at FTO, while holes are transferred to the α-Fe2O3 nanobranches that serve as charge mediators to the electrolyte. The morphology of α-Fe2O3 that varies from ultrathin nanoflakes to nanorod/nanofiber structures depending on the Fe precursor concentration was shown to have a significant impact on the photo-induced activity of the α-Fe2O3/TiO2 composites. In particular, it is shown that for an optimized photo-electrochemical structure, a combination of critical factors should be achieved such as (i) TiO2 light absorption and photo-activation vs.α-Fe2O3-induced shadowing effect and (ii) the availability of free TiO2 surface vs.α-Fe2O3-coated surface. Finally, theoretical analysis, based on DFT calculations, confirmed the optical properties experimentally determined for the α-Fe2O3/TiO2 hierarchical nanostructures. We anticipate that this new multi-step hydrothermal process can be a blueprint for the design and development of other hierarchical heterogeneous metal oxide electrodes suitable for photo-electrochemical applications.
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In this paper, we establish connections between the thresholds and mechanisms of the damage and white-light generation upon femtosecond laser irradiation of wide-bandgap transparent materials. On the example of Corning Willow glass, evolution of ablation craters, their quality, and white-light emission were studied experimentally for 130-fs, 800-nm laser pulses. The experimental results indicate co-existence of several ablation mechanisms which can be separated in time. Suppression of the phase explosion mechanism of ablation was revealed at the middle of the irradiation spots. At high laser fluences, air ionization was found to strongly influence ablation rate and quality and the main mechanisms of the influence are analysed. To gain insight into the processes triggered by laser radiation in glass, numerical simulations have been performed with accounting for the balance of laser energy absorption and its distribution/redistribution in the sample, including bremsstrahlung emission from excited free-electron plasma. The simulations have shown an insignificant role of avalanche ionization at such short durations of laser pulses while pointing to high average energy of electrons up to several dozens of eV. At multi-pulse ablation regimes, improvement of crater quality was found as compared to single/few pulses.
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Multipartite entanglement and nonclassicality of four-mode Gaussian states generated in two simultaneous nonlinear processes involving parametric down-conversion and frequency up-conversion are analyzed assuming the vacuum as the initial state. Suitable conditions for the generation of highly entangled states are found. Transfer of the entanglement from the down-converted modes into the up-converted ones is also suggested. The analysis of the whole set of states reveals that sub-shot-noise intensity correlations between the equally-populated down-converted modes, as well as the equally-populated up-converted modes, uniquely identify entangled states. They represent a powerful entanglement identifier also in other cases with arbitrarily populated modes.
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The dynamics of intense twin beams in pump-depleted parametric down-conversion is studied. A generalized parametric approximation is suggested to solve the quantum model. Its comparison with a semiclassical model valid for larger twin-beam intensities confirms its applicability. The experimentally observed maxima in the spectral and spatial intensity auto- and cross- correlation functions depending on pump power are explained in terms of different speeds of the (back-) flow of energy between the individual down-converted modes and the corresponding pump modes. This effect is also responsible for the gradual replacement of the initial exponential growth of the down-converted fields by the linear one. Furthermore, it forms a minimum in the curve giving the effective number of twin-beam modes. These effects manifest a tight relation between the twin-beam coherence and its internal structure, as clearly visible in the model. Multiple maxima in the intensity correlation functions originating in the oscillations of energy flow between the pump and down-converted modes are theoretically predicted.
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Nonclassicality criteria based on intensity moments and derived from the usual matrix approach are compared to those provided by the majorization theory. The majorization theory is shown to give a greater number of more suitable nonclassicality criteria. Fifteen experimentally useful criteria of the majorization theory containing the intensity moments up to the fifth order are identified. Their performance is experimentally demonstrated on the set of eleven potentially nonclassical states generated from a twin beam by postselection based on detecting a given number of photocounts in one arm by using an iCCD camera.
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Spatial and spectral coherence of high-intensity twin-beam states propagating from the near-field to the far-field configurations is experimentally investigated by measuring intensity auto- and cross-correlation functions. The experimental setup includes a moving crystal and an iCCD camera placed at the output plane of an imaging spectrometer. Evolution from the tight near-field spatial position cross-correlations to the far-field momentum cross-correlations, accompanied by changeless spectral cross-correlations, is observed. Intensity autocorrelation functions and beam profiles are also monitored as they provide the number of degrees of freedom constituting the down-converted beams. The strength of intensity cross-correlations as an alternative quantity for the determination of the number of degrees of freedom is also measured. The relation between the beam coherence and the number of degrees of freedom is discussed.
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It is shown that spatial correlation functions measured for correlated photon pairs at the single-photon level correspond to speckle patterns visible at high intensities. This correspondence is observed for the first time in one experimental setup by using different acquisition modes of an intensified CCD camera in low and high intensity regimes. The behavior of intensity auto- and cross-correlation functions in dependence on pump-beam parameters including power and transverse profile is investigated.
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States with sub-Poissonian photon-number statistics obtained by post-selection from twin beams are experimentally generated. States with Fano factors down to 0.62 and mean photon numbers around 12 are reached. Their quasi-distributions of integrated intensities attaining negative values are reconstructed. An intensified CCD camera with a quantum detection efficiency exceeding 20% is utilized both for post-selection and beam characterization. Experimental results are compared with theory that provides the optimum experimental conditions.
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A method for the determination of absolute quantum detection efficiency is suggested based on the measurement of photocount statistics of twin beams. The measured histograms of joint signal-idler photocount statistics allow us to eliminate an additional noise superimposed on an ideal calibration field composed of only photon pairs. This makes the method superior above other approaches presently used. Twin beams are described using a paired variant of quantum superposition of signal and noise.
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Surface spontaneous parametric down-conversion is predicted as a consequence of continuity requirements for electric- and magnetic-field amplitudes at a discontinuity of chi;{(2)} nonlinearity. A generalization of the usual two-photon spectral amplitude is suggested to describe this effect. Examples of nonlinear layered structures and periodically poled nonlinear crystals show that surface contributions to spontaneous down-conversion can be important.
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A balanced homodyne detection scheme with nanosecond time resolution and sub-shot-noise sensitivity has been developed and successfully tested yielding an efficient detection scheme for high-speed quantum-optical measurements and communication protocols, for example, quantum cryptography. The parameters of the detector and its precise balancing allow complete characterization of quantum states created by femtosecond light pulses that include the measurement of photon number, optical phase, and statistical properties with a high signal-to-noise ratio for the whole bandwidth from DC to several tens of megahertz. The electronic part of the detector is based on a commercially available amplifier that provides ease of construction and use while yielding good performance.