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Nature Communications

Generation of photonic entanglement in green fluorescent proteins

Siyuan Shi, Prem Kumar, Kim Fook Lee

Published Nov 29, 2017• 23 citations
Publisher

Abstract

Recent development of spectroscopic techniques based on quantum states of light can precipitate many breakthroughs in observing and controlling light-matter interactions in biological materials on a fundamental quantum level. For this reason, the generation of entangled light in biologically produced fluorescent proteins would be promising because of their biocompatibility. Here we demonstrate the generation of polarization-entangled two-photon state through spontaneous four-wave mixing in enhanced green fluorescent proteins. The reconstructed density matrix indicates that the entangled state is subject to decoherence originating from two-photon absorption. However, the prepared state is less sensitive to environmental decoherence because of the protective β-barrel structure that encapsulates the fluorophore in the protein. We further explore the quantumness, including classical and quantum correlations, of the state in the decoherence environment. Our method for photonic entanglement generation may have potential for developing quantum spectroscopic techniques and quantum-enhanced measurements in biological materials.

DOI
10.1038/s41467-017-02027-9

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Recent development of spectroscopic techniques based on quantum states of light can precipitate many breakthroughs in observing and controlling light-matter interactions in biological materials on a fundamental quantum level. For this reason, the generation of entangled light in biologically produced fluorescent proteins would be promising because of their biocompatibility. Here we demonstrate the generation of polarization-entangled two-photon state through spontaneous four-wave mixing in enhanced green fluorescent proteins. The reconstructed density matrix indicates that the entangled state is subject to decoherence originating from two-photon absorption. However, the prepared state is less sensitive to environmental decoherence because of the protective β-barrel structure that encapsulates the fluorophore in the protein. We further explore the quantumness, including classical and quantum correlations, of the state in the decoherence environment. Our method for photonic entanglement generation may have potential for developing quantum spectroscopic techniques and quantum-enhanced measurements in biological materials.
Recent studies in quantum biology suggest that quantum mechanics help us to explore quantum processes in biological system. Here, we demonstrate generation of photon pairs through spontaneous four-wave mixing process in naturally occurring fluorescent proteins. We develop a general empirical method for analyzing the relative strength of nonlinear optical interaction processes in five different organic fluorophores. Our results indicate that the generation of photon pairs in green fluorescent proteins is subject to less background noises than in other fluorophores, leading to a coincidence-to-accidental ratio ~145. As such proteins can be genetically engineered and fused to many biological cells, our experiment enables a new platform for quantum information processing in a biological environment such as biomimetic quantum networks and quantum sensors.
Fluorescence microscopy has become integral to biological studies for the technique’s ability to elucidate structures of biomolecules for in-situ studies with high selectivity and specificity. Imaging of intrinsic indicators, such as fluorescent amino acids in proteins, provides important information, but can be challenging to accomplish. Current microscopy techniques that measure native fluorescence without the use of exogenous labels involve either direct UV excitation which is commonly non-localized and can be detrimental to the system, or multiphoton absorption which must be conducted at high intensities, therefore posing high risks of photodamage. As such, we seek to investigate an efficient way to gently excite native fluorescence in biological systems in a way that overcomes these limitations. Quantum entangled photon pairs generated via spontaneous parametric downconversion (SPDC), may be an alternative to conducting two-photon absorption (TPA) to excite fluorescence in amino acids without the high fluences currently used. These photon pairs are highly correlated in time. Thus, the arrival of one photon is simultaneously followed by the arrival of its sister photon. As a result, a molecule interacting with the photon pair should simultaneously absorb both photons, leading to a linear two-photon absorption rate, and the linearity of the two-photon process should dramatically reduce the light intensity necessary for TPA. Therefore, quantum entangled photon pairs offer the possibility of performing low intensity UV excitation using photons in the visible wavelength range. With this work, we generated and characterized entangled photons generated via SPDC, and investigated whether fluorescent amino acids can be excited, and the subsequent fluorescence induced with entangled two-photon absorption. Results show that much higher entangled two-photon rates than what are currently available are needed to measure significant signals with entangled two-photon excitation.
Abstract Entangled photons with time-energy correlations are predicted to have improved sensitivity compared with classical light in two-photon fluorescence, which is promising for lowering the phototoxicity in biomedical imaging. While the mechanism has been demonstrated in atoms and crystals, the effectiveness in biological molecules has been under debate. Here we report the experimental results, including both positive and negative ones, in various samples. While entanglement induced enhancement in the sum frequency generation of a nonlinear crystal was confirmed, we observe no such enhancement in the two-photon nonlinear process of various molecules. However, we observed classical two-photon fluorescence excited by nW light in rare earth element doped core-shell structure nano-crystals, which can also be used in sensitive biomedical imaging. Our results provide guidance in characterizing the effect of entanglement in two-photon processes.