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.
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.
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.
Recently, there has been significant interest in multiple-parameter quantum estimation techniques that exploit quantum resources. In particular, the estimation of optical transmission is a crucial parameter in various scientific fields and industries. In optical-based sensing, precision can be enhanced through two approaches: increasing the number of photons that interact with the samples and utilizing quantum states of light. In this paper, we investigate multiple transmission estimation using bright two-mode squeezed states (bTMSSs), which combine the advantages of both bright light and quantum states. We calculate the precision bound for multiple transmission estimation by employing multiple copies of bTMSSs with experimentally feasible optimal measurement, determining both the quantum Cramer-Rao bound and the Cramer-Rao bound. Our results demonstrate that multiple copies of bTMSSs can achieve quantum-enhanced sensitivity for multiple transmissions compared to coherent states, and the ultimate limit of precision can be attained in regions with high nonlinear gain. Furthermore, as an application, we show the quantum-enhanced sensing in circular dichroism sensing using a pair of bTMSSs. Our strategy for multiple transmission estimation offers a practical platform for exploring real-world quantum sensing applications.
We address the precise characterization of coupling strength of nonlinear media in continuous-variable (CV) quantum systems using coherent and squeezed vacuum states as Gaussian probes, together with their photon-added and photon-subtracted counterparts as non-Gaussian probes. We consider three main classes of nonlinear Hamiltonians, namely quadrature nonlinearities, generalized squeezing and Kerr-type interactions. By analytically evaluating the quantum Fisher information (QFI), we compare the performance of Gaussian and non-Gaussian probes and assess the optimal probe based on the probe parameters, energy resource and non-Gaussianity. Our results are twofold as follows: first, for coherent-state family, the improvement provided by photon addition at fixed coherent amplitude originates mainly from the extra energy carried by the probe and does not provide a genuine metrological resource, since the same precision can be achieved by a Gaussian coherent-state signal of a larger energy, which can be more easily produced. Second, in contrast, photon addition and subtraction become effective resources when applied to already nonclassical states such as squeezed vacuum states. In this case, they lead to a significant enhancement of the QFI, particularly for higher-order interactions. Although Gaussian squeezed states remain optimal at equal energy constraint, photon-added and photon-subtracted squeezed states achieve comparable sensitives with significantly lower squeezing requirements. Since large squeezing level remains experimentally challenging, these non-Gaussian probes offer a practical route towards enhanced estimation of the nonlinear coupling strength within currently accessible squeezing regimes.
Enhancing the precision of a measurement requires maximizing the information that can be gained about the quantity of interest from probing a system. For optical-based measurements, such an enhancement can be achieved through two approaches, increasing the number of photons used to interrogate the system and using quantum states of light to increase the amount of quantum Fisher information gained per photon. Here we consider the use of quantum states of light with a large number of photons, namely the bright single-mode squeezed state and the bright two-mode squeezed state, which take advantage of both of these approaches for the problem of transmission estimation. We show that, in the limit of large squeezing, these states approach the maximum possible quantum Fisher information per photon for transmission estimation that is achieved with the Fock state and the vacuum two-mode squeezed state. Since the bright states we consider can be generated at powers much higher than those of the quantum states that achieve the maximum quantum Fisher information per photon, they can achieve a much higher absolute precision as quantified by the quantum Cram\'er-Rao bound. We discuss the effects of losses external to the system on the precision of transmission estimation and identify simple measurement techniques that can saturate the quantum Cram\'er-Rao bound for the bright squeezed states even in the presence of such external losses.
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 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.