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Analytical Chemistry

Optical Absorption Measurements with Parametric Down-Converted Photons

Zhi Gao Zhao, Kent A. Meyer, William Barclay Whitten, Robert W. Shaw

Published Aug 26, 2008• 3 citations
Publisher

Abstract

It has been known for some time that correlated detection of pairs of photons generated by parametric down-conversion can eliminate several sources of error that occur in single-beam measurements. In the correlated photon measurements, the down-converted photons are separated into two beams with one photon of a pair in each beam. The absolute detection efficiency of a detector in one beam can be determined from the count rate of a detector in the other beam and the coincidence rate for the two detectors. These ideas can be used to measure the optical absorbance of a sample placed in front of one of the detectors. Errors due to stray light and dark counts are substantially reduced and fluctuations in pump intensity largely eliminated.

DOI
10.1021/ac800911t

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It has been known for some time that correlated detection of pairs of photons generated by parametric down-conversion can eliminate several sources of error that occur in single-beam measurements. In the correlated photon measurements, the down-converted photons are separated into two beams with one photon of a pair in each beam. The absolute detection efficiency of a detector in one beam can be determined from the count rate of a detector in the other beam and the coincidence rate for the two detectors. These ideas can be used to measure the optical absorbance of a sample placed in front of one of the detectors. Errors due to stray light and dark counts are substantially reduced and fluctuations in pump intensity largely eliminated.
Taking advantage of our previous experimental results and calculations that establish a new approach to the calibration of photo detectors using correlated photon pairs, we developed an experimental setup with a fast electronic control unit for the direct measurement of photon statistics. The most convenient source for generating such correlated photon pairs is a nonlinear optical process of spontaneous parametric down conversion (SPDC). When a photon of the pump beam is incident to a nonlinear crystal with phase matching condition, a pair of photons (signal and idler) is created at the same time. The photons are detected in the signal beam, and a controllable shutter is placed in the idler beam. When a detection event is made in the signal beam the fast optical shutter opens for a certain (pre-programmed) time. While the opening time of the shutter is adjustable with good time resolution, the time interval between the photons in the idler beam can be scanned, so the photon statistics can be determined.
We have developed our pervious experimental setup using correlated photon pairs (to the calibration of photo detectors) to realize a controllable photon source. For the generation of such photon pairs we use the non-linear process of parametric down conversion. When a photon of the pump beam is incident to a nonlinear crystal with phase matching condition, a pair of photons (signal and idler) is created at the same time with certain probability. We detect the photons in the signal beam with a single photon counting module (SPCM), while delaying those in the idler beam. Recently we have developed a fast electronic unit to control an optical shutter (a Pockels cell) placed to the optical output of the idler beam. When we detect a signal photon with the controlling electronic unit we are also able to open or close the fast optical shutter. Thus we can control which idler photons can propagate through the Pockels cell. So with this photon source we are able to program the number of photons in a certain time window. This controllable photon source that is able to generate a known number of photons with specified wavelength, direction, and polarization could be useful for applications in high-accuracy optical characterisation of photometric devices at the ultra-low intensities. This light source can also serve as a standard in testing of optical image intensifiers, night vision devices, and in the accurate measurement of spectral distribution of transmission and absorption in optical materials.
Photon correlated beams, generated by parametric down-conversion in nonlinear crystals (PDC), have been proved successfully for the measurement of quantum efficiency, of single photon detectors [1, 2, 3, 4] and can be used for measuring transmittance, as well. The main feature relies on the realization of two correlated quantum channels yielding coincident events. To reduce uncertainty [4, 5, 6] and determine its ultimate limit, contributions to statistical noise in a real experimental set-up are here investigated, and a general model is proposed to calculate the maximum likelihood best estimators and evaluate the probability of coincidence. In typical measurement scheme a channel is set as trigger (idler, i) and attention is paid to catch at least the same amount of correlated photons in the other channel (signal, s) [4]. Unwanted uncorrelated photons due to PDC itself result in a decreased degree of correlation, noise fluctuations in coincidence measurements and asymmetry between the two channels, whose mean photon rate can be quite different. We indicate by with the mean rate of correlated photons in s and i channels We address the total mean photon rates in both channels as where terms take into account also additive background photon rates due to straylight and detector noise. Actually statistical noise is also due to losses of correlated photons by optical elements, non ideal detectors and electronic devices in both channels. We distinguish, therefore, between optical losses ( transmittance of the correlated photon path), detection losses detectorquantum efficiency), electronic losses associated to the dead times time during which the detection system is unable to detect photons). It is usual to identify dead times as non-extending and extending: in the first case, all photons following a revealed photon within the fixed time interval are ignored, while in the second case any incoming photon produces or prolongs Eventually the finite duration of the time coincidence window, modifies the distribution probability of coincident events. Let us consider the distribution probability of single channel
Efficient Generation of Entangled Photon-Pairs The first experiments with correlated photons have been performed in the context of EPR-Bell experiments on the realistic and local properties of quantum mechanics. The source used there produced pairs of polarization entangled photons from a 2-photon decay of Calcium atoms. The technical requirements of these experiments were high (vacuum systems, stronge dye-lasers, etc.) whereas the efficiency of the source was quite low. An important step forward was the introduction of spontaneous parametric down conversion (SPDC), which has become the most common source in quantum optics for generating correlated or entangled photon pairs. In this process photons of an intense pump laser convert to photon pairs in an optical nonlinear crystal. Conservation of energy and momentum leads to strong correlations between the generated photons. With this kind of two-photon source it was possible to realize or improve many experiments on the foundations of quantum mechanics addressing the EPR-Paradoxon and in the new field of quantum information. But again, more advanced experiments and applications suffer from the limited ef- ficiency of the fluorescence process. Many photon pairs are lost by spatial and spectral filtering, which is necessary to achieve polarization entanglement and long coherence times. Different techniques have been implemented to increase the number of photon pairs using two-crystal arrangements, focusing techniques or periodically poled crystals. Most of these methods have the disadvantage that no entangled photons have been observed. It is the aim of this work to increase the yield and to improve the mode definition of entangled photon pairs generated by resonant enhancement of the pump mode and the fluorescence modes. As a first step a linear cavity for the pump mode was realized. Since the conversion probability is proportional to the pump power it was possible to increase the photon pair count rate by factor of 7 over the previous source. Besides the possibility of further improvement on already established pair correlation experiments, such an enhancement allows to build a compact source for photon pairs, in which an expensive argon-ion laser is replaced by a cheap diode laser. Among other applications such sources are of strong interest for quantum cryptography. 3 In many quantum information experiments optical fibers are use to carry the photons over long distance. Therefore, light from the parametric down-conversion source has to be efficiently coupled into fibers. In the second part we report on a new method to optimize collection efficiency by matching the angular distribution of the parametric fluorescence to the spatial mode of an optical fiber. By using this technique, we detected 366500 polarization-entangled photon pairs per second in the near-infrared region in single-mode optical fibers for 465 mW pump power (at 351.1 nm) with a 2 mm BBOcrystal. The entanglement of the photon pairs was verified by measuring polarization correlations of more than 96% in a HV-basis and in a ±45◦-basis. To our knowledge, such enormous count rates of highly entangled photon pairs have not been reached yet with any other technique. In the third part of this thesis we investigated the process of parametric downconversion in a cavity which is resonant to certain longitudinal down-conversion modes only. The idea of placing the parametric down-conversion source inside a cavity is not new. Such a device is usually referred to as a single or double resonant optical parametric oscillator (OPO) and is mainly used to generate squeezed quantum states. In that kind of application the system is operating close to but still under the threshold of oscillation. In our application the situation is quite different. The system is operating far below threshold so that mainly spontaneous emission occurs. In that mode correlations between single photons can still be observed. But bouncing the light back and forth inside the cavity increases the interaction length and hence enhances the signal levels of the down-conversion fields. Further, by resonating two certain modes only, the bandwidth is reduced by orders of magnitude and the coherence time is found to be inverse proportional to the bandwidth. A similar experiment has already been realized with a type-I parametric down-converter in the resonator. We have tried to realize a compact double resonant OPO far below threshold with a type-II parametric down-converter in a high-finesse cavity to realize a bright source of entangled photon pairs with extremely narrow bandwidth.