Entangled photons can encode more information than classical light, enabling quantum-enhanced optical measurements. We formulate optical rotatory dispersion (ORD) spectroscopy as a quantum metrology phase-estimation problem using photons entangled in their orbital angular momentum (OAM). While polarization-entangled photons have previously been shown to improve the precision of ORD measurements, we extend this approach by exploiting the higher-dimensional entanglement available through photon OAM. We show how the optical activity of a medium can be imprinted on the interference patterns of OAM-entangled photons measured by coincidence detection. The attainable precision of this setup, quantified by the Fisher information, exceeds that of the classical detection scheme. Our analysis shows that the metrological performance is controlled by the symmetry of the entangled state, the OAM index through the Gouy phase accumulated in the detection geometry, and the pixel resolution of the detectors. Beyond chiroptical spectroscopy, our results provide a general strategy for the broader task of phase estimation with entangled structured light.
Entangled photons can encode more information than classical light, enabling quantum-enhanced optical measurements. We formulate optical rotatory dispersion (ORD) spectroscopy as a quantum metrology phase-estimation problem using photons entangled in their orbital angular momentum (OAM). While polarization-entangled photons have previously been shown to improve the precision of ORD measurements, we extend this approach by exploiting the higher-dimensional entanglement available through photon OAM. We show how the optical activity of a medium can be imprinted on the interference patterns of OAM-entangled photons measured by coincidence detection. The attainable precision of this setup, quantified by the Fisher information, exceeds that of the classical detection scheme. Our analysis shows that the metrological performance is controlled by the symmetry of the entangled state, the OAM index through the Gouy phase accumulated in the detection geometry, and the pixel resolution of the detectors. Beyond chiroptical spectroscopy, our results provide a general strategy for the broader task of phase estimation with entangled structured light.
The phenomenon of molecular optical activity manifests itself as the rotation of the plane of linear polarization when light passes through chiral media. Measurements of optical activity and its wavelength dependence, that is, optical rotatory dispersion, can reveal information about intricate properties of molecules, such as the three-dimensional arrangement of atoms comprising a molecule. Given a limited probe power, quantum metrology offers the possibility of outperforming classical measurements. This has particular appeal when samples may be damaged by high power, which is a potential concern for chiroptical studies. We present the first experiment in which multiwavelength polarization-entangled photon pairs are used to measure the optical activity and optical rotatory dispersion exhibited by a solution of chiral molecules. Our work paves the way for quantum-enhanced measurements of chirality, with potential applications in chemistry, biology, materials science, and the pharmaceutical industry. The scheme that we use for probing wavelength dependence not only allows one to surpass the information extracted per photon in a classical measurement but also can be used for more general differential measurements.
Orbital angular momentum (OAM) as both classical and quantum states of light has proven essential in numerous applications, from high-capacity information transfer to enhanced precision and accuracy in metrology. Here, we extend OAM metrology to relativistic scenarios to determine the Lorentz factor of a moving reference frame, exploiting the fact that OAM is not Lorentz invariant. We show that the joint OAM spectrum from entangled states is modified by length contraction when measured by two observers moving relative to the entanglement source. This relative motion rescales the spatial dimensions, thus breaking the orthogonality of the OAM measurement process and resulting in a broadening of the joint OAM spectrum that can precisely determine the Lorentz factor. We experimentally simulate velocities up to 0.99c, confirm the predicted broadening, and use the measurement outcomes to extract the Lorentz factor. Our work provides a pathway for novel measurement techniques suitable for relativistic conditions that leverage OAM structured light as a resource.
The bandwidth of any communication system, classical or quantum, is limited by the number of orthogonal states in which the information can be encoded. Quantum key distribution systems available commercially rely on the two-dimensional polarisation state of photons. Quantum computation has also been largely designed on the basis of qubits. However, a photon is endowed with other degrees of freedom, such as orbital angular momentum (OAM). OAM is an attractive basis to be used for quantum information because it is discrete and theoretically infinite-dimensional. This promises a higher information capacity per photon which can lead to more complex quantum computation protocols and more security and robustness for quantum cryptography. Entanglement of OAM naturally arises from spontaneous parametric down-conversion (SPDC). However, any practical experiment utilising the innately high-dimensional entanglement of the orbital angular momentum (OAM) state space of photons is subject to the modal capacity of the detection system. Only a finite subset of this space is accessible experimentally. Given such a constraint, we show that the number of measured, entangled OAM modes in photon pairs generated by SPDC can be increased by tuning the phase-matching conditions in the SPDC process. We achieve this by tuning the orientation angle of the nonlinear crystal generating the entangled photons.
Photons with a twisted phase front carry a quantized amount of orbital angular momentum (OAM) and have become important in various fields of optics, such as quantum and classical information science or optical tweezers. Because no upper limit on the OAM content per photon is known, they are also interesting systems to experimentally challenge quantum mechanical prediction for high quantum numbers. Here, we take advantage of a recently developed technique to imprint unprecedented high values of OAM, namely spiral phase mirrors, to generate photons with more than 10,000 quanta of OAM. Moreover, we demonstrate quantum entanglement between these large OAM quanta of one photon and the polarization of its partner photon. To our knowledge, this corresponds to entanglement with the largest quantum number that has been demonstrated in an experiment. The results may also open novel ways to couple single photons to massive objects, enhance angular resolution, and highlight OAM as a promising way to increase the information capacity of a single photon.
Orbital angular momentum (OAM) is one of the most recently discovered properties of light, and it is only in the past decade its quantum properties have been the subject of experimental investigations and have found applications. Unlike polarization, which is only bidimensional, orbital angular momentum provides, with relative ease, unprecedented access to a theoretically unbounded discrete state space. The process of spontaneous parametric down-conversion has long been used as a source of two-photon states that can be entangled in several degrees of freedom, including OAM. In this thesis, the properties of the natural OAM spectrum associated with the entangled states produced by parametric down-conversion were investigated. Chapters 2 and 3 describe the production and detection of tunable high-dimensional OAM entanglement in a down-conversion system. By tuning the phase-matching conditions and improving the detection stage, a substantial increase in the half-width of the OAM correlation spectrum was observed. The conjugate variable of OAM, angular position, was also considered when examining high-dimensional states entangled in OAM. In order to efficiently determine their dimension, high-dimensional entangled states were probed by implementing a technique based on phase masks composed of multiple angular sectors, as opposed to narrow single-sector analysers. Presented in chapter 4, this technique allows the measurements of tight angular correlations while maintaining high optical throughput. The states so produced were then used for a number of applications centred around the concept of mutually unbiased bases. One can define sets of mutually unbiased bases for arbitrary subspaces of the OAM state space. Two bases are mutually unbiased if the measurement of a state in one basis provides no information about the state as described in the other basis. Complete measurements in mutually unbiased bases of high-dimensional OAM spaces are presented in chapter 5. Measurements in sets of mutually unbiased bases are integral to quantum science and can be used in a variety of protocols that fully exploit the large size of the OAM state space; we describe their use in efficient quantum state tomography, quantum key distribution and entanglement detection. Caution is however necessary when dealing with state spaces embedded in higher-dimensional spaces, such as that provided by OAM. Experimental tests of Bell-type inequalities allow us to rule out local hidden variable theories in the description of quantum correlations. Correlations inconsistent with the states observed, or even with quantum mechanics, known as super-quantum correlations, have however been recorded previously in experiments that fail to comply with the fair-sampling conditions. Chapter 6 describes an experiment that uses a particular choice of transverse spatial modes for which super-quantum correlations persist even if the detection is made perfectly efficient. The sets of modes carrying OAM allow a complete description of the transverse field. The ability to control and combine additional degrees of freedom provides the possibility for richer varieties of entanglement and can make quantum protocols more powerful and versatile. One such property of light, associated with transverse modes possessing radial nodes in the field distribution, can be accessed within the same type of experimental apparatus used for OAM. In chapter 7, the radial degree of freedom is explored, together with OAM, in the context of Hong-Ou-Mandel interference.
Photons are an ideal candidate for encoding both classical and quantum information. Besides spin angular momentum associated with circular polarization, single photon can also carry other fundamentally new degree of freedom of orbital angular momentum related to the spiral phase structure of light. The key significance of orbital angular momentum lies in its potential in realizing a high-dimensional Hilbert space and in encoding a high-dimensional quantum information. Since Allen et al. [Allen L, Beijersbergen M W, Spreeuw R J C, Woerdman J P 1992 Phys. Rev. A 45 8185] recognized the physical reality of photon orbital angular momentum in 1992, rapidly growing interest has been aroused in orbital angular momentum (OAM) from both classical and quantum points of view. Here we present an overall review on the high-order orbital angular momentum of photon, including its preparation and manipulation based on some specific techniques and also its applications. The spatial light modulator is a commercial device that has been widely employed to generate the OAM beams. We make and identify the optical OAM superposition with very high quantum numbers up to l=360. Recently, the metallic spiral phase mirrors were also developed to produce high-order OAM beams up to l=5050. In addition, the Q-plates made of anisotropic and inhomogeneous liquid crystals were invented to generate high-order OAM beams in a polarization-controllable manner, and the OAM superposition of l=± 50 were achieved. Owing to high rotational symmetry, these high OAM beams have been found to have more and more important applications in the fields of high-sensitivity sensing and high-precision measurements. Two fascinating examples are discussed in detail. The first example is that the research group led by Prof. Zeilinger has prepared and observed the quantum entanglement of high orbital angular momenta up to l=±300 by the technique of polarization-OAM entanglement swapping, and they demonstrated that the angular resolution could be significantly improved by a factor of l. Their result was the first step for entangling and twisting even macroscopic, spatially separated objects in two different directions. The second example is that the research group led by Prof. Padgett has demonstrated an elegant experiment of rotational Doppler effects for visible light with l=±20 OAM superposition. They showed that a spinning object with an optically rough surface might induce a Doppler effect in light reflected from the direction parallel to the rotation axis, and the frequency shift was proportional to both the disk's angular speed and the optical OAM. The potential applications in noncontact measurement of angular speed and in significant improvement of angular resolution for remote sensing will be particularly fascinating.