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Physical Review A

Effects of time-energy correlation strength in molecular entangled photon spectroscopy

Fabiano Lever, Sven Ramelow, Markus Gühr

Published Nov 20, 2019• 8 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.100.053844

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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.
Polarization-entangled photon pairs can be efficiently prepared into pure Bell states with a high fidelity via type-II spontaneous parametric down-conversion (SPDC) of narrow-band pump light. However, the use of femtosecond pump pulses to generate multiphoton states with precise timing often requires spectral filtering to maintain a high quality of polarization entanglement. This typically reduces the efficiency of photon pair collection. We experimentally map the polarization correlations of photon pairs from such a source over a range of down-converted wavelengths with a high spectral resolution and find strong polarization correlations everywhere. A spectrally dependent imbalance between contributions from the two possible decay paths of SPDC is identified as the reason for a reduction in entanglement quality observed with femtosecond pump pulses. Our spectral measurements allow us to predict the polarization correlations for arbitrary filter profiles when the frequency degree of freedom of the photon pairs is ignored.
Classical time-resolved optical spectroscopy experiments are performed using sequences of ultrashort light pulses, with photon fluxes incident on the sample which are many orders of magnitude higher than real-world conditions corresponding to sunlight illumination. Here we overcome this paradigm by exploiting quantum correlations to perform time-resolved spectroscopy with entangled photons. Starting from spontaneous parametric down-conversion driven by a continuous-wave laser, we exploit the temporal entanglement between randomly generated signal/idler pairs to obtain temporal resolution, and their spectral entanglement to select the excitation frequency. We also add spectral resolution in detection, using a Fourier transform approach which employs a common-path interferometer. We demonstrate the potential of our entangled-photon streak camera by resolving, at the single-photon level, excitation energy transfer cascades from LH2 to LH1 in the photosynthetic membrane and disentangling the lifetimes of two dyes in a mixture. We show that time-resolved spectroscopy with quantum light can be performed without compromising measurement time, recording a fluorescence time trace in less than a minute even for samples with low quantum yield, which can be reduced to sub-second times with acceptable signal-to-noise ratio. Our results provide a new approach to ultrafast optical spectroscopy, where experiments are performed under conditions comparable to real-world sunlight illumination.
We report on experimental measurements of coincidence and single particle spectral shapes of biphoton signals when frequency entangled states are generated by SPDC crystals pumped by short pulses.It is shown evidence for biphoton coincidence spectrum narrower and single-particle one wider than the pump spectrum, with a large contrast between coincidence and singles distributions.The investigation of biphoton correlations has been performed by fixing one monochromator at the maximal transmission wavelength on down-converted signal gate and scanning the one placed in the idler branch in order to observe the spectral distribution of single counts and coincidences.The degree of entanglement is evaluated by the ratio of the FWHM of single particle and coincidence distributions: the greater the ratio, the greater is the entanglement.The degree of entanglement in frequency variables can be very high: it increases linearly with the length of the crystal, and decreases with the growing pump pulse.
Squeezed photons, which provide a quantum-correlated light with reduced noise, have emerged as a powerful resource for sensing the structures of matter. Here, we study the pump-probe scheme using squeezed photons whose spectral correlation of amplitudes can be tailored. A microscopic theory reveals a highly time-energy-resolved signal that is not attainable by classical pump-probe scheme. The results show high selectivity of accessing the molecular correlation functions, e.g., suppression of ground-state bleaching signal, and can significantly enhance signal intensity that surpasses the bottleneck by entangled twin photons. An application to a monolayer semiconductor model reveals a real-time monitoring of valley excitons and their dynamics, i.e., conversion between dark and bright excitons. We further show the intermediate squeezing regime-not strong squeezing-where time-resolved spectroscopy is favorable. Our work offers a paradigm for studying nonequilibrium dynamics of matter, in photocatalysis and optoelectronics.
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.
Entangled photons have attracted increasing interest as resources for developing time-resolved spectroscopic techniques. Theoretical studies suggest that their non-classical correlations enable time-resolved spectroscopy with monochromatic pumping and can selectively isolate specific Liouville pathways in nonlinear optical signals. In an earlier study, we proposed a fluorescence detection scheme that could, in principle, be implemented using existing single-photon detectors [Y. Fujihashi et al., Sci. Adv. 12, eaed7026 (2026)]. In that design, the time origin was defined by detecting the arrival of the pulsed laser used to pump the nonlinear crystal for spontaneous parametric down-conversion, a requirement that made the overall experiment cumbersome. This study theoretically examines an alternative protocol that defines the reference time based on the arrival of idler photons. We demonstrate that this idler-referenced scheme functions effectively when the entangled photons exhibit either negative or negligible frequency correlations. Eliminating the pump-timing channel simplifies the optical layout and lowers the experimental barrier to realizing time-resolved two-dimensional fluorescence spectroscopy with entangled photons. Although the photons may exhibit frequency correlations in isolation, their frequency-time degrees of freedom can behave as effectively uncorrelated when considered over the full measurement timescale. Therefore, fully exploiting non-classical correlations requires an entangled photon source whose temporal characteristics are carefully matched to the overall timescale of the experiment.