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We investigate the precision of estimating the interaction strength between a two-level system (TLS) and a single-photon pulse when the latter is subject to chirping. We consider linear, quadratic, and sinusoidal temporal phases applied to Gaussian and exponential temporal profiles. At the asymptotic time, when the TLS has fully decayed to its ground state, the fundamental precision depends solely on the magnitude of its spectral amplitude. For quadratically phase-modulated Gaussian pulses, this is entirely determined by the spectral bandwidth. We provide expressions for evaluating the fundamental precision for general temporal profiles and phase modulations. Finally, we show that experimentally feasible mode-resolved measurements are optimal, or close to it, for chirped, pulsed single photon spectroscopy.

It depends. For a single molecule interacting with one mode of a biphoton probe, we show that the spectroscopic information has three contributions, only one of which is a genuine two-photon contribution. When all the scattered light can be measured, solely this contribution exists and can be fully extracted using unentangled measurements. Furthermore, this two-photon contribution can, in principle, be matched by an optimised but unentangled single-photon probe. When the matter system spontaneously emits into inaccessible modes, an advantage due to entanglement can not be ruled out. In practice, time-frequency entanglement does enhance spectroscopic performance of the oft-studied weakly-pumped spontaneous parametric down conversion (PDC) probes. For two-level systems and coupled dimers, more entangled PDC probes yield more spectroscopic information, even in the presence of emission into inaccessible modes. Moreover, simple, unentangled measurements can capture between 60% - 90% of the spectroscopic information. We thus establish that biphoton spectroscopy using source-engineered PDC probes and unentangled measurements can provide tangible quantum enhancement. Our work underscores the intricate role of entanglement in single-molecule spectroscopy using quantum light., Comment: 18+14 pages, 12+14 figures, 1+0 tables

We study the fundamental limits of the precision of estimating parameters of a quantum matter system when it is probed by a travelling pulse of quantum light. In particular, we focus on the estimation of the interaction strength between the pulse and a two-level atom, equivalent to the estimation of the dipole moment. Our analysis of single-photon pulses highlights the interplay between the information gained from the absorption of the photon by the atom as measured in absorption spectroscopy, and the perturbation to the temporal mode of the photon due to spontaneous emission. Beyond the single-photon regime, we introduce an approximate model to study more general states of light in the limit of short pulses, where spontaneous emission can be neglected. We also show that for a vast class of entangled biphoton states, quantum entanglement between the signal mode interacting with the atom and the idler mode provides no fundamental advantage and the same precision can be obtained with a separable state. We conclude by studying the estimation of the electric dipole moment of a sodium atom using quantum light. Our work initiates a quantum information theoretic methodology for developing the theory and practice of quantum light spectroscopy., Comment: v2: 30 pages, 10 figures, Fig. 7 fixes an error in Fig. 8 of v1, appendix E replaces appendix B of v1

We present a model-independent measure of dynamical complexity based on simulating complex quantum dynamics using stroboscopic Markovian dynamics. Tools from classical signal processing enable us to infer the Hilbert space dimension of a complex quantum system evolving under a time-independent Hamiltonian via pulsed interrogation. We evaluate our model-independent simulation complexity (MISC) for the spin-boson model and simulated third-order pump-probe spectroscopy data for exciton transport in coupled dimers with vibrational levels. The former provides insights into coherence and population dynamics in the two-level system while the latter reveals the dimension of the singly-excited manifold of the dimer. Finally, we probe the complexity of excitonic transport in light harvesting 2 (LH2) and Fenna-Matthews-Olson (FMO) complexes using data from two recent nonlinear ultrafast optical spectroscopy experiments. For the latter we make some model-independent inferences that are commensurate with model-specific ones. This includes estimating the fewest number of parameters needed to fit the experimental data and identifying the spatial extent, i.e., delocalization size, of quantum states occurring in this complex quantum dynamics., Comment: 21 pages, inculding 6 appendices and 10 figures

In recent years, exploring the possible use of separable states as resource for achieving quantum information processing(QIP) tasks has been gaining increasing significance. In this context, a particularly important demonstration has been that non-vanishing discord is the necessary condition for the separable states to be used as resource for remotely preparing any arbitrary pure target state [Nature Physics $8$, $666$ $(2012)$]. The present work stems from our observation that not only resource states with same discord can imply different efficiencies (in terms of average fidelity) of the remote state preparation (RSP) protocol, but also states with higher discord can imply lower RSP efficiency. This, therefore, necessitates identification of the relevant feature of quantum correlations which can appropriately quantify effectiveness of the resource state for the RSP protocol. To this end, for the two-qubit Bell-diagonal states, we show that an appropriate measure of simultaneous correlations in three mutually unbiased bases can serve to quantify usefulness of the resource for the RSP task using entangled as well as separable states, including non-discordant states as resource. In particular, it is revealed that zero-discord states having such non-vanishing measure can be useful for remotely preparing a subset of pure target states. Thus, this work shows that, using separable states, an effective resource for QIP tasks such as RSP can be provided by simultaneous correlations in mutually unbiased bases., Comment: 7 pages

The present work is motivated by the question as to what aspect of correlation entailed by the two-qubit state serves as the appropriate quantitative resource for steering. To this end, considering Bell-diagonal states, suitable measures of simultaneous correlations in two and three complementary (mutually unbiased) bases are identified as the relevant resources for quantum steering. Quantitative relations between appropriate measures of quantum steering and the corresponding measures of simultaneous correlations in complementary bases are demonstrated which ensure that for two qubit steerable Bell-diagonal states, higher value of simultaneous correlations in mutually unbiased bases necessarily implies higher degree of quantum steering, both for two and three setting steering scenarios., Comment: 5 pages, accepted version

The hitherto unexplored nonlocality of quantum correlations in the information transfer protocol of remote state preparation (RSP) is investigated in terms of a unified nonlocality argument formulated for teleportation as well as for two distinct RSP schemes. The argument differs only in the respective types of local measurements used in each scenario. One of the RSP schemes uses single particle projective measurements, while the other uses joint Bell-basis measurements. Interestingly, the quantum mechanical violations of the Bell-CHSH type inequalities formulated for each of the RSP setups, while being equal to each other, also turn out to be equal to that of the corresponding Bell-CHSH type local realist inequality for teleportation, using the common resource of non-maximally entangled state. This reveals that for such a resource state, the maximum amount of extractable nonlocality of correlations involved in the transfer of information is the same for the standard teleportation protocol and the two RSP schemes considered here, thereby implying that the essential difference between teleportation and remote state preparation lies in the amount of classical information required to be exchanged between parties, and not in the nonlocality of underlying correlations., Comment: 9 pages, 1 figure