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arXiv:2108.13970 · Physical Review A

Quantum Fisher information bounds on precision limits of circular dichroism

Jiaxuan Wang, G. S. Agarwal

Published Dec 16, 2021• 10 citations
arXivHTMLPDF

Abstract

Circular dichroism is a widely used technique for investigating optically chiral molecules, especially for biomolecules. It is thus of great importance that these parameters be estimated precisely so that the molecules with desired functionalities can be designed. In order to surpass the limits of classical measurements, we need to probe the system with quantum light. We develop the quantum Fisher information matrix (QFIM) for precision estimates of the circular dichroism and the optical rotary dispersion for a variety of input quantum states of light that are easily accessible in the laboratory. The Cramer-Rao bounds for all four chirality parameters are obtained from the QFIM for (a) single photon input states with a specific linear polarization and for (b) NOON states having two photons with both either left polarized or right polarized. The QFIM bounds, using quantum light, are compared with bounds obtained for classical light beams, i.e., beams in coherent states. Quite generally, both the single-photon state and the NOON state exhibit superior precision in the estimation of absorption and phase shift in relation to a coherent source of comparable intensity, especially in the weak-absorption regime. In particular, the NOON state naturally offers the best precision among the three. We compare QFIM bounds with the error sensitivity bounds, as the latter are relatively easier to measure whereas the QFIM bounds require full state tomography.

DOI
10.1103/physreva.104.062613

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Circular dichroism is a widely used technique for investigating optically chiral molecules, especially for biomolecules. It is thus of great importance that these parameters be estimated precisely so that the molecules with desired functionalities can be designed. In order to surpass the limits of classical measurements, we need to probe the system with quantum light. We develop the quantum Fisher information matrix (QFIM) for precision estimates of the circular dichroism and the optical rotary dispersion for a variety of input quantum states of light that are easily accessible in the laboratory. The Cramer-Rao bounds for all four chirality parameters are obtained from the QFIM for (a) single photon input states with a specific linear polarization and for (b) NOON states having two photons with both either left polarized or right polarized. The QFIM bounds, using quantum light, are compared with bounds obtained for classical light beams, i.e., beams in coherent states. Quite generally, both the single-photon state and the NOON state exhibit superior precision in the estimation of absorption and phase shift in relation to a coherent source of comparable intensity, especially in the weak-absorption regime. In particular, the NOON state naturally offers the best precision among the three. We compare QFIM bounds with the error sensitivity bounds, as the latter are relatively easier to measure whereas the QFIM bounds require full state tomography.
The measurement of circular dichroism (CD) has widely been exploited to distinguish the different enantiomers of chiral structures. It has been applied to natural materials (e.g., molecules) as well as to artificial materials (e.g., nanophotonic structures). However, especially for chiral molecules the signal level is very low and increasing the signal-to-noise ratio is of paramount importance to either shorten the necessary measurement time or to lower the minimum detectable molecule concentration. As one solution to this problem, we propose here to use quantum states of light in CD sensing to reduce the noise below the shot noise level encountered when using coherent states of light. Through a multiparameter estimation approach, we identify the ultimate quantum limit of the precision in CD sensing, allowing for general schemes including additional ancillary modes. We show that the ultimate quantum limit can be achieved by various optimal schemes. These include using a pair of Fock-state probes in a direct sensing configuration and pairs of twin beams in an ancilla-assisted sensing configuration, for both of which photon number-resolved detection is shown to be the optimal measurement. These optimal schemes offer a significant quantum enhancement even in the presence of some additional system loss. The near optimality of a scheme using a single twin beam in a direct sensing configuration is also shown for cases where the actual CD signal is very small. Alternative optimal schemes involving single-photon sources and detectors are also proposed. This work paves the way for further investigations of quantum metrological techniques in chirality sensing.
The concentration of a chiral solution is a key parameter in many scientific fields and industrial processes. This parameter can be estimated to high precision by exploiting circular birefringence or circular dichroism present in optically active media. Using the quantum Fisher information formalism, we quantify the performance of Gaussian probes in estimating the concentration of chiral analytes. We find that bright-polarization squeezed state probes provide a quantum advantage over equally bright classical strategies that scales exponentially with the squeezing factor for a circularly birefringent sample. Four-fold precision enhancement is achievable using state-of-the-art squeezing levels and intensity measurements.
In recent times there has been growing interest in Raman optical activity (ROA) for its label free detection of absolute configuration, conformation, and stereochemical structure in chiral biosamples and drug molecules. Since ROA signals are generally small, techniques such as stimulation by a probe beam can be used to enhance the signal strength. However, with a classical probe, the measurement precision is still fundamentally limited by its shot noise. To solve this problem we propose the use of two-mode squeezed vacuum and show that it can achieve sub-shot noise limited measurement sensitivity. Using quantum estimation theory, we derived the quantum Fisher information and the quantum Cramér-Rao bound (QCRB) for stimulated ROA measurement to quantify the precision enhancement. This improvement comes from photon-number correlations which suppress the intensity fluctuation common to both modes. We further show that balanced detection of the output intensity difference is a practical measurement scheme that approaches the QCRB and becomes optimal in the small-chirality limit. This opens a promising path toward more sensitive Raman chiroptical spectroscopy of weak and photosensitive samples.
The fundamental precision limit of an interferometer is crucial since it bounds the best possible sensitivity one could achieve using such a device. This thesis will focus on several different interferometers and try to give the ultimate precision bounds by carefully counting all the resources used in the interferometers. The thesis begins with the basics of the quantum state of light. The fundamentals of quantum metrology are also reviewed and discussed. More specifically, the terminology of classical and quantum Cram\'er-Rao bound and classical and quantum Fisher information are introduced. Chapter 3 discusses the conclusive precision bounds in two-mode interferometer such as Mach-Zehnder interferometer (MZI) and SU(1,1) interferometer. I revisit the quantum Fisher information approach of these two interferometers and show the discrepancy of phase sensitivity on the physically same setup. Then I establish fundamental precision estimation bounds for such device, due to the reason that many works of literature fail to accurately count the resources and knowledge of phase-to-be-estimated used in the interferometers. The analysis suggests that for a MZI, one can never do better than SNL in phase sensitivity, when an input to one of the two ports is the vacuum. If one does not allow the detector to use any external phase reference or power resource, then the precision is limited by the SNL. For a SU(1,1) interferometer, firstly, when one of the input states is restricted to be a vacuum state, I showed that by using either the phase-averaging method or the quantum Fisher information matrix method, different phase configurations of the SU(1,1) interferometer result in the same QFI. Secondly, I compared the results of the phase-averaging method and the quantum Fisher information matrix method, and then I argued that for an SU(1,1) interferometer, phase averaging or quantum Fisher information matrix method is generally required, and they are equivalent. Finally, I used the quantum Fisher information matrix method to calculate the precision limit for other common input states, such as two coherent state inputs or coherent state with squeezed vacuum inputs. In chapter 4, I will consider a passive multi-mode interferometer for multiparameter phase estimation. It was suggested that optical networks with relatively inexpensive overhead---single photon Fock states, passive optical elements, and single photon detection---can show significant improvements over classical strategies for single-parameter estimation, when the number of modes in the network is small. In this chapter, I analytically compute the quantum Cramer-Rao bound to show these
As a method to extract information from optical systems, imaging can be viewed as a parameter estimation problem. The fundamental precision in locating one emitter or estimating the separation between two incoherent emitters is bounded below by the multiparameter quantum Cramér-Rao bound (QCRB). Multiparameter QCRB gives an intrinsic bound in parameter estimation. We determine the ultimate potential of quantum-limited imaging for improving the resolution of a far-field, diffraction-limited optical field within the paraxial approximation. We show that the quantum Fisher information matrix (QFIm) in about one emitter’s position is independent on its true value. We calculate the QFIm of two unequal-brightness emitters’ relative positions and intensities; the results show that only when the relative intensity and centroids of two-point sources, including longitudinal and transverse directions, are known exactly, the separation in different directions can be estimated simultaneously with finite precision. Our results give the upper bounds on certain far-field imaging technology and will find wide use in applications from microscopy to astrometry.
Abstract The quantum Cramér–Rao bound sets a fundamental limit on the accuracy of unbiased parameter estimation in quantum systems, relating the uncertainty in determining a parameter to the inverse of the quantum Fisher information. We experimentally demonstrate near saturation of the quantum Cramér–Rao bound in the phase estimation of a solid-state spin system, provided by a nitrogen-vacancy center in diamond. This is achieved by comparing the experimental uncertainty in phase estimation with an independent measurement of the related quantum Fisher information. The latter is independently extracted from coherent dynamical responses of the system under weak parametric modulations, without performing any quantum-state tomography. While optimal parameter estimation has already been observed for quantum devices involving a limited number of degrees of freedom, our method offers a versatile and powerful experimental tool to explore the Cramér–Rao bound and the quantum Fisher information in systems of higher complexity, as relevant for quantum technologies.