Periodic Reporting for period 4 - LightNet (LightNet - Tracking the Coherent Light Path in Photosynthetic Networks)
Okres sprawozdawczy: 2020-07-01 do 2021-12-31
Nature has developed photosynthesis to power life. Networks of light harvesting antennas capture the sunlight to funnel the photonic energy towards reaction centres. Surprisingly, quantum coherences are observed in the energy transfer of photosynthetic complexes, even at room temperature.
Does nature exploit quantum concepts? Does the coherence help to find an optimal path for robust or efficient transfer? How are the coherences sustained? What is their spatial extent in a real light-harvesting network? So far only solutions of complexes were studied, far from the natural network operation, putting on hold conclusions as to a biological role of the coherences.
At the start of this project my group had succeeded in the first detection of coherent oscillations of a single photo-synthetic complex at physiological conditions, and non-classical photon emission of individual complexes. These pioneering results, together with our expertise in nanophotonics, gave the way to address photosynthetic networks in real nano-space and on femtosecond timescale. Specific objectives addressed:
1. Ultrafast single protein detection: tracing the fs coherent energy transfer path of an individual complex; addressing the very nature of the persistent coherences.
2. Beyond fluorescence: light harvesting complex are designed for light transport, not emission. I will explore innovative alternatives: optical antennas to enhance quantum efficiency; detection of stimulated emission; and electrical read-out on graphene.
3. Nanoscale light transport: using local excitation and detection by nanoholes, nanoslits and scanning antenna probes I will spatially map the extent of the inter-complex transfer.
4. The network: combining both coherent fs excitation and localized nanoscale excitation/detection I will track the extent of coherences throughout the network.
The impact of this first exploration of light transport in a nanoscale bionetwork ranges to solar energy management, molecular biology, polymer chemistry and material science.
Does nature exploit quantum concepts? Does the coherence help to find an optimal path for robust or efficient transfer? How are the coherences sustained? What is their spatial extent in a real light-harvesting network? So far only solutions of complexes were studied, far from the natural network operation, putting on hold conclusions as to a biological role of the coherences.
At the start of this project my group had succeeded in the first detection of coherent oscillations of a single photo-synthetic complex at physiological conditions, and non-classical photon emission of individual complexes. These pioneering results, together with our expertise in nanophotonics, gave the way to address photosynthetic networks in real nano-space and on femtosecond timescale. Specific objectives addressed:
1. Ultrafast single protein detection: tracing the fs coherent energy transfer path of an individual complex; addressing the very nature of the persistent coherences.
2. Beyond fluorescence: light harvesting complex are designed for light transport, not emission. I will explore innovative alternatives: optical antennas to enhance quantum efficiency; detection of stimulated emission; and electrical read-out on graphene.
3. Nanoscale light transport: using local excitation and detection by nanoholes, nanoslits and scanning antenna probes I will spatially map the extent of the inter-complex transfer.
4. The network: combining both coherent fs excitation and localized nanoscale excitation/detection I will track the extent of coherences throughout the network.
The impact of this first exploration of light transport in a nanoscale bionetwork ranges to solar energy management, molecular biology, polymer chemistry and material science.
Main project results (see full report below for details):
- Single light harvesting complex excitation spectroscopy
- Room temperature excitation-emission spectra of single LH2 complexes reveal disorder
- Time traces of the anti-bunching [g(2)(0)] and single emitter character on single LH2 complexes
- Spectral phase control has no effects on the emission of single LH2 complexes
- Control of vibronic transition rates by resonant single-molecule-nanoantenna coupling
- Transient ultrafast “encoded” spectroscopy on a single molecule (DBT)
- Stimulated emission microscopy of single emitters (nanocrystals)
- Stimulated emission set-up with sensitivity of 10E-7 differential signal, sufficient to see stimulated emission of individual Quntum dots, yet not of a single organic dye molecule (DBT)
- Closed loop coherent control loop on a single emitter (quantum dot two-photon excitation)
- Spectral phase control of non-linear nanoantenna excitation
- First detection of single FMO complexes at room temperature
- Anti-bunching of single FMO enhanced by resonant nanoantenna
- Photocurrent-detected 2D electronic spectroscopy to reveal energy transfer in light harvesting
- Scanning antenna probe imaging of LH2
- Fabrication of 2-5 nm gap-antennas with the new Zeiss ORION He-ion-microscope
- Room temperature strong coupling (~100meV) of dye molecules and LH2 in antenna nanogaps
- Non-fluorescent, interferometric scattering detection of single proteins with ~15kD sensitivity
- Development of In-line Balanced Interferometric Scattering detection in an associated ERC-PoC project (IBIS)
- Widefield phase imaging to track and discriminate nanoparticles
- Development ultrafast transient holographic microscopy to track nanoparticle fs transients
- Tracking fluorescently labelled vesicles in a cell using interferometric widefield imaging
- Spatio-temporal imaging of light transport on LH nanotubes
- Spatio-temporal mapping of energy diffusion in Au, Si, graphene
- Diffusion of emission in an LH2 membrane, over 300 - 500nm.
Exploitation and dissemination:
The project did result in a patent on interferometric scattering detecting of single proteins, allowing a shot-noise limited sensitivity down to 15kD; the same was supported by an ERC-PoC grant connected to this AdvGrant project.
The project has resulted in around 40 publications (and still a few pending on 2021 research results) in Web-of-Science journals: in Science, Nature NanoTechnol., Nature Phot., Science Adv., Angew.Chem. Adv.Mat. ACSNano, even 11 papers in NanoLetters, 4 in JPC.Lett. etc, etc.…. In parallel the project was presented at many international conferences, workshops, discussion and science management meetings, in total around 60 times. Unfortunately, in the last two years 2020-2021, dissemination was handicapped by COVID, with many scheduled meetings and invitations being canceled. Highlights of the project were picked up in 9 news items and press releases.
- Single light harvesting complex excitation spectroscopy
- Room temperature excitation-emission spectra of single LH2 complexes reveal disorder
- Time traces of the anti-bunching [g(2)(0)] and single emitter character on single LH2 complexes
- Spectral phase control has no effects on the emission of single LH2 complexes
- Control of vibronic transition rates by resonant single-molecule-nanoantenna coupling
- Transient ultrafast “encoded” spectroscopy on a single molecule (DBT)
- Stimulated emission microscopy of single emitters (nanocrystals)
- Stimulated emission set-up with sensitivity of 10E-7 differential signal, sufficient to see stimulated emission of individual Quntum dots, yet not of a single organic dye molecule (DBT)
- Closed loop coherent control loop on a single emitter (quantum dot two-photon excitation)
- Spectral phase control of non-linear nanoantenna excitation
- First detection of single FMO complexes at room temperature
- Anti-bunching of single FMO enhanced by resonant nanoantenna
- Photocurrent-detected 2D electronic spectroscopy to reveal energy transfer in light harvesting
- Scanning antenna probe imaging of LH2
- Fabrication of 2-5 nm gap-antennas with the new Zeiss ORION He-ion-microscope
- Room temperature strong coupling (~100meV) of dye molecules and LH2 in antenna nanogaps
- Non-fluorescent, interferometric scattering detection of single proteins with ~15kD sensitivity
- Development of In-line Balanced Interferometric Scattering detection in an associated ERC-PoC project (IBIS)
- Widefield phase imaging to track and discriminate nanoparticles
- Development ultrafast transient holographic microscopy to track nanoparticle fs transients
- Tracking fluorescently labelled vesicles in a cell using interferometric widefield imaging
- Spatio-temporal imaging of light transport on LH nanotubes
- Spatio-temporal mapping of energy diffusion in Au, Si, graphene
- Diffusion of emission in an LH2 membrane, over 300 - 500nm.
Exploitation and dissemination:
The project did result in a patent on interferometric scattering detecting of single proteins, allowing a shot-noise limited sensitivity down to 15kD; the same was supported by an ERC-PoC grant connected to this AdvGrant project.
The project has resulted in around 40 publications (and still a few pending on 2021 research results) in Web-of-Science journals: in Science, Nature NanoTechnol., Nature Phot., Science Adv., Angew.Chem. Adv.Mat. ACSNano, even 11 papers in NanoLetters, 4 in JPC.Lett. etc, etc.…. In parallel the project was presented at many international conferences, workshops, discussion and science management meetings, in total around 60 times. Unfortunately, in the last two years 2020-2021, dissemination was handicapped by COVID, with many scheduled meetings and invitations being canceled. Highlights of the project were picked up in 9 news items and press releases.
Most approaches used in this project are state-of-the-art: such as, Transient ultrafast “encoded” spectroscopy on a single molecule; Stimulated emission microscopy of singles; Photocurrent-detected 2D electronic spectroscopy; Scanning antenna probe imaging; Fabrication of 2-5 nm gap-antennas by He-ion-microscopy; Anti-bunching of single proteins; In-line Balanced Interferometric Scattering detection of proteins; Ultrafast transient holographic microscopy; Spatio-temporal imaging of light transport. At the end of the project several expected results are pretty much along the defined objectives, yet more interestingly and importantly equally many novel results were not foreseen and are purely result of the insights developed throughout the project