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arXiv:2307.02204 · Quantum Science and Technology

Does entanglement enhance single-molecule pulsed biphoton spectroscopy?

Aiman Khan, Francesco Albarelli, Animesh Datta

Published Mar 12, 2024• 12 citations
arXivHTMLPDF

Abstract

Abstract 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% and 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.

DOI
10.1088/2058-9565/ad331b

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Abstract 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% and 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.
In this paper, we explore the time-energy domain quantum-classical transition comparing a classical pump-probe experiment on a diatomic molecule to its quantum enhanced counterpart, where the pump and probe pulses are substituted by the signal and idler beams of a spontaneous parametric down conversion (SPDC) source. Absorption of biphotons generated with SPDC exploits quantum time-energy entanglement to enhance the overall yield and selectivity of the process, when compared with a classical pump-probe setup, while maintaining femtosecond time resolution. We systematically study the effects of correlation strength on process efficiency and selectivity, comparing the results to classical pump-probe spectra. An excitation scheme to improve the yield based on spectral narrowing of biphotons is shown. The results indicate that the quantum improvements in yield are caused by a more efficient use of the total power available for the process.
Entangled photons carry nontrivial quantum correlations that defy classical physics and provide new tools for monitoring quantum dynamics in molecules. The use of low-flux entangled photons in molecular spectroscopy has been proposed in the past to probe excited-state dynamics with enhanced temporal and spectral resolutions. However, these techniques have been challenging to implement experimentally since the resulting signal has a low signal-to-noise ratio. The signal strength can be boosted by using intense entangled-photon beams, where multiple pairs of entangled photons are present in the environment. This allows the molecule under study to interact with both entangled and unentangled photons, where the classical component of the spectroscopic signal stemming from the latter can mask the spectral features associated with the former. In this Letter, we show how the signal arising from unentangled photons can be eliminated when intense entangled-photon beams are used in two-dimensional electronic spectroscopy (2DES), and demonstrate the advantage of photonic entanglement.
The true role of entanglement in two-photon virtual-state spectroscopy (Saleh et al 1998 Phys. Rev. Lett. 80 3483), a two-photon absorption spectroscopic technique that can retrieve information about the energy level structure of an atom or a molecule, is controversial. The consideration of closely related techniques, such as multidimensional pump–probe spectroscopy (Roslyak et al 2009 Phys. Rev. A 79 , 063409), suggests that spectroscopic information might also be retrieved by using uncorrelated pairs of photons. Here we show that this is not the case. In the two-photon absorption process, the ability to obtain information about the energy level structure of a medium depends on the spectral shape of existing temporal (frequency) correlations between the absorbed photons. In fact, it is a combination of both the presence of frequency correlations (entanglement) and their specific spectral shape that makes the realization of two-photon virtual-state spectroscopy possible. This result helps in selecting the type of two-photon source that needs to be used in order to experimentally perform the two-photon virtual-state spectroscopy technique.
Recent advances in techniques for generating quantum light have stimulated research on novel spectroscopic measurements using quantum entangled photons. One such spectroscopy technique utilizes non-classical correlations among entangled photons to enable measurements with enhanced sensitivity and selectivity. Here, we investigate the spectroscopic measurement utilizing entangled three photons. In this measurement, time-resolved entangled photon spectroscopy with monochromatic pumping [A. Ishizaki, J. Chem. Phys. 153, 051102 (2020)] is integrated with the frequency-dispersed two-photon counting technique, which suppresses undesired accidental photon counts in the detector and thus allows one to separate the weak desired signal. This time-resolved frequency-dispersed two-photon counting signal, which is a function of two frequencies, is shown to provide the same information as that of coherent two-dimensional optical spectra. The spectral distribution of the phase-matching function works as a frequency filter to selectively resolve a specific region of the two-dimensional spectra, whereas the excited-state dynamics under investigation are temporally resolved in the time region longer than the entanglement time. The signal is not subject to Fourier limitations on the joint temporal and spectral resolution, and therefore, it is expected to be useful for investigating complex molecular systems in which multiple electronic states are present within a narrow energy range.
Quantum light is increasingly recognized as a promising resource for developing optical measurement techniques. Particular attention has been paid to enhancing the precision of the measurements beyond classical techniques by using nonclassical correlations between quantum entangled photons. Recent advances in the quantum optics technology have made it possible to manipulate spectral and temporal properties of entangled photons, and photon correlations can facilitate the extraction of matter information with relatively simple optical systems compared to conventional schemes. In these respects, the applications of entangled photons to time-resolved spectroscopy can open new avenues for unambiguously extracting information on dynamical processes in complex molecular and materials systems. Here, we propose time-resolved spectroscopy in which specific signal contributions are selectively enhanced by harnessing nonclassical correlations of entangled photons. The entanglement time characterizes the mutual delay between an entangled twin and determines the spectral distribution of photon correlations. The entanglement time plays a dual role as the knob for controlling the accessible time region of dynamical processes and the degrees of spectral selectivity. In this sense, the role of the entanglement time is substantially equivalent to the temporal width of the classical laser pulse. The results demonstrate that the application of quantum entangled photons to time-resolved spectroscopy leads to monitoring dynamical processes in complex molecular and materials systems by selectively extracting desired signal contributions from congested spectra. We anticipate that more elaborately engineered photon states would broaden the availability of quantum light spectroscopy.
The utility of quantum light as a spectroscopic tool is demonstrated for frequency-dispersed pump-probe, integrated pump-probe, and two-photon fluorescence signals which show Ramsey fringes. Simulations of the frequency-dispersed transmission of a broadband pulse of entangled photons interacting with a three-level model of matter reveal how the non-classical time-bandwidth properties of entangled photons can be used to disentangle congested spectra, and reveal otherwise unresolved features. Quantum light effects are most pronounced at weak intensities when entangled photon pairs are well separated, and are gradually diminished at higher intensities when different photon pairs overlap.