Professor Jenny Clark
School of Mathematical and Physical Sciences
Head of Materials and Biological Physics Research Cluster
Professor of Materials Physics
+44 114 222 3526
Full contact details
School of Mathematical and Physical Sciences
D16
Hicks Building
Hounsfield Road
Sheffield
S3 7RH
- Profile
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My research interests involve understanding the photophysics of carbon-based materials such as biological materials, organic semiconductors and graphene.
I do this using a variety of spectroscopic techniques. For more information see my personal webpage or contact me.
Research Experience
- 2009-2013 Royal Society Dorothy Hodgkin Fellow, Cambridge University, UK.
- 2009 Visiting Scholar, Hyderabad University, India.
- 2007-2009 Postdoctoral Research Fellow, Politecnico di Milano, Italy.
Supervisor: Prof. Guglielmo Lanzani
Fellowships and Awards
- 2014 University of Sheffield Vice-Chancellor's Fellowship (5 years).
- 2010 Charles and Catherine Darwin Research Fellowship (3 years).
- 2009 Royal Society Dorothy Hodgkin Fellowship (4 years).
- 2004 European Materials Research Society (E-MRS) student award.
- 2003 EPSRC PhD studentship and Industrial Case Award (Seiko Epson UK, 3 years).
Career Breaks
- 2012 Maternity leave (9 months)
- 2013 Maternity leave (13 months)
- Qualifications
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- 2003-2007 PhD in Physics, Cambridge University, UK. Supervisor: Prof. C. Silva.
- 1999-2003 MSci in Physics with a Year in Europe, Imperial College, London, UK. (First Class Degree)
- Research interests
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New laser facility at Sheffield university
The University of Sheffield has a new laser facility that I help run. The facility is currently being built and will have several spectroscopy stations including:
- Pump-probe spectroscopy in the UV/VIs-NIR with 10fs resolution, capable of tracking excited-state dynamics up to 1ms.
- Time-resolved IR spectroscopy and 2D IR spectroscopy
- Time-resolved Raman
- Photoluminescence Up-Conversion
Ultrafast spectroscopy of carbon-based materials
To study organic semiconductors and biological samples, we mainly use transient absorption spectroscopy.
This technique uses laser pulses as short as 7 femtoseconds (7 millionths of a billionth of a second) to take snapshots of the electronic and vibrational state of the molecules after they have absorbed light.
By delaying the time at which the 'probe' pulse arrives to take a snapshot of the molecule, we can track the dynamics of the electrons in the molecule as a function of time.
- Publications
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Show: Featured publications All publications
Featured publications
Journal articles
- Spin Statistics for Triplet–Triplet Annihilation Upconversion: Exchange Coupling, Intermolecular Orientation, and Reverse Intersystem Crossing. JACS Au, 1(12), 2188-2201.
- Emissive spin-0 triplet-pairs are a direct product of triplet–triplet annihilation in pentacene single crystals and anthradithiophene films. Nature Chemistry, 13(2), 163-171.
- Manipulating molecules with strong coupling: harvesting triplet excitons in organic exciton microcavities. Chemical Science, 11(2), 343-354. View this article in WRRO
- Triplet-pair states in organic semiconductors. Annual Review of Physical Chemistry, 70(1), 323-351.
- The Nature of Singlet Exciton Fission in Carotenoid Aggregates. Journal of the American Chemical Society, 137(15), 5130-5139. View this article in WRRO
- Triplet Dynamics in Pentacene Crystals: Applications to Fission-Sensitized Photovoltaics. Advanced Materials, 26(6), 919-924.
- Ultrafast Long-Range Charge Separation in Organic Semiconductor Photovoltaic Diodes. Science, 343(6170), 512-516.
All publications
Journal articles
- Twisted Carotenoids Do Not Support Efficient Intramolecular Singlet Fission in the Orange Carotenoid Protein.. J Phys Chem Lett, 6135-6142.
- Spin Statistics for Triplet–Triplet Annihilation Upconversion: Exchange Coupling, Intermolecular Orientation, and Reverse Intersystem Crossing. JACS Au, 1(12), 2188-2201.
- In optimized rubrene-based nanoparticle blends for photon upconversion, singlet energy collection outcompetes triplet-pair separation, not singlet fission. Journal of Materials Chemistry C.
- Emissive spin-0 triplet-pairs are a direct product of triplet–triplet annihilation in pentacene single crystals and anthradithiophene films. Nature Chemistry, 13(2), 163-171.
- Author Correction: Emissive spin-0 triplet-pairs are a direct product of triplet–triplet annihilation in pentacene single crystals and anthradithiophene films (Nature Chemistry, (2020), 10.1038/s41557-020-0593-y). Nature Chemistry.
- A Thermostable Protein Matrix for Spectroscopic Analysis of Organic Semiconductors. Journal of the American Chemical Society, 142(32), 13898-13907. View this article in WRRO
- Metal–organic framework nanosheets for enhanced performance of organic photovoltaic cells. Journal of Materials Chemistry A. View this article in WRRO
- Manipulating molecules with strong coupling: harvesting triplet excitons in organic exciton microcavities. Chemical Science, 11(2), 343-354. View this article in WRRO
- A hybrid organic–inorganic polariton LED. Light: Science & Applications, 8(1). View this article in WRRO
- Heavy-atom effects on intramolecular singlet fission in a conjugated polymer. The Journal of Chemical Physics, 151(4).
- Triplet-pair states in organic semiconductors. Annual Review of Physical Chemistry, 70(1), 323-351.
- Strong coupling in a microcavity containing β-carotene. Optics Express, 26(3), 3320-3327. View this article in WRRO
- The entangled triplet pair state in acene and heteroacene materials. Nature Communications, 8. View this article in WRRO
- Intermolecular states in organic dye dispersions: excimers vs. aggregates. Journal of Materials Chemistry C, 5, 8380-8389. View this article in WRRO
- Efficient Radiative Pumping of Polaritons in a Strongly Coupled Microcavity by a Fluorescent Molecular Dye. Advanced Optical Materials, 4(10), 1615-1623. View this article in WRRO
- Polaritons: Efficient Radiative Pumping of Polaritons in a Strongly Coupled Microcavity by a Fluorescent Molecular Dye (Advanced Optical Materials 10/2016). Advanced Optical Materials, 4(10), 1614-1614. View this article in WRRO
- The Nature of Singlet Exciton Fission in Carotenoid Aggregates. Journal of the American Chemical Society, 137(15), 5130-5139. View this article in WRRO
- Humidity, light and temperature dependent characteristics of Au/N-BuHHPDI/Au surface type multifunctional sensor. Sensors and Actuators B: Chemical, 192, 565-571.
- Triplet Dynamics in Pentacene Crystals: Applications to Fission-Sensitized Photovoltaics. Advanced Materials, 26(6), 919-924.
- Ultrafast Long-Range Charge Separation in Organic Semiconductor Photovoltaic Diodes. Science, 343(6170), 512-516.
- Temperature-Independent Singlet Exciton Fission in Tetracene. Journal of the American Chemical Society, 135(44), 16680-16688.
- Activated Singlet Exciton Fission in a Semiconducting Polymer. Journal of the American Chemical Society, 135(34), 12747-12754.
- Control of Intrachain Charge Transfer in Model Systems for Block Copolymer Photovoltaic Materials. Journal of the American Chemical Society, 135(13), 5074-5083.
- Femtosecond torsional relaxation. Nature Physics, 8(3), 225-231.
- Giant broadband nonlinear optical absorption response in dispersed graphene single sheets. Nature Photonics, 5(9), 554-560.
- Ultrafast Dynamics of Exciton Fission in Polycrystalline Pentacene. Journal of the American Chemical Society, 133(31), 11830-11833.
- Two-Photon Poly(phenylenevinylene) DFB Laser†. Chemistry of Materials, 23(3), 805-809.
- Stimulated emission and ultrafast optical switching in a ter(9,9′-spirobifluorene)-co -methylmethacrylate copolymer. Journal of Polymer Science Part B: Polymer Physics, 49(1), 52-61.
- Organic photonics for communications. Nature Photonics, 4(7), 438-446.
- Gain and ultrafast optical switching in PMMA optical fibers and films doped with luminescent conjugated polymers and oligomers. Frontiers of Optoelectronics in China, 3(1), 45-53.
- Femtosecond laser fabrication of microfluidic channels for organic photonic devices. Applied Optics, 48(31), G114-G114.
- Determining exciton bandwidth and film microstructure in polythiophene films using linear absorption spectroscopy. Applied Physics Letters, 94(16), 163306-163306.
- Determining exciton coherence from the photoluminescence spectral line shape in poly(3-hexylthiophene) thin films. The Journal of Chemical Physics, 130(7), 074904-074904.
- Ultrafast optofluidic gain switch based on conjugated polymer in femtosecond laser fabricated microchannels. Applied Physics Letters, 94(4), 041123-041123.
- Charge recombination in distributed heterostructures of semiconductor discotic and polymeric materials.. Journal of Applied Physics, 103(12), 124510-124510.
- Blue polymer optical fiber amplifiers based on conjugated fluorene oligomers. Journal of Nanophotonics, 2(1), 023504-023504.
- Macrocyclic Parallel Dimer Showing Quantum Coherence of Quintet Multiexcitons at Room Temperature. Journal of the American Chemical Society.
- Radiative pumping in a strongly coupled microcavity filled with a neat molecular film showing excimer emission. Physical Chemistry Chemical Physics.
- Exploring the Versatile Uses of Triplet States: Working Principles, Limitations, and Recent Progress in Phosphorescence, TADF, and TTA. ACS Applied Optical Materials.
- Excitonic organic materials for photochemical and optoelectronic applications: general discussion. Faraday Discussions.
- Conjugation-length dependence of regioregular oligo 3-alkyl(thienylene-vinylene)s demonstrates polyene-like behaviour with weak electron–electron correlations. Physical Chemistry Chemical Physics.
- Singlet fission is incoherent in pristine orthorhombic single crystals of rubrene: no evidence of triplet-pair emission. Faraday Discussions.
- Metal‐Organic Framework Nanosheets as Templates to Enhance Performance in Semi‐Crystalline Organic Photovoltaic Cells. Advanced Science, 2200366-2200366.
- Ultrafast optical gain switch in organic photonic devices. J. Mater. Chem., 20(3), 519-523.
- Role of Intermolecular Coupling in the Photophysics of Disordered Organic Semiconductors: Aggregate Emission in Regioregular Polythiophene. Physical Review Letters, 98(20).
- Molecular-weight dependence of interchain polaron delocalization and exciton bandwidth in high-mobility conjugated polymers. Physical Review B, 74(11).
- Spin statistics for triplet-triplet annihilation upconversion: exchange coupling, intermolecular orientation and reverse intersystem crossing.
Chapters
- Pump-push-probe transient spectroscopy of isolated conjugated oligomers, Springer Series in Chemical Physics (pp. 463-465).
Conference proceedings papers
- A tale of two triplets: manipulating and harvesting triplet pairs with strong light-matter coupling (Conference Presentation). Physical Chemistry of Semiconductor Materials and Interfaces XVII, 19 August 2018 - 23 August 2018.
- Ultrafast Long-Range Charge Separation in Organic Semiconductor Photovoltaic Diodes. 19th International Conference on Ultrafast Phenomena, 2014.
- Plastic optical fibres dopants to obtain gain enlargement and ultrafast optical switching. International Conference on Applications of Optics and Photonics
- Chip cracks during assembly: Finding and eliminating the critical defect. 2011 IEEE 61st Electronic Components and Technology Conference (ECTC), 31 May 2011 - 3 June 2011.
- Use of wafer backside inspection and SPR to address systemic tool and process issues. Metrology, Inspection, and Process Control for Microlithography XXIV
- Investigation of Local Dynamics on the Sub-micron Scale in Organic Blends Using an Ultrafast Confocal Microscope. MRS Proceedings, Vol. 1270
- Nanoscale Imaging of the Interface Dynamics in Polymer Blends by Femtosecond Pump-Probe Confocal Microscopy. International Conference on Ultrafast Phenomena, 2010.
- Organic optofluidic devices produced by femtosecond laser micromachining. 2009 International Symposium on Optomechatronic Technologies, 21 September 2009 - 23 September 2009.
- Ultrafast Confocal Microscope for Functional Imaging of Organic Thin Films (pp 161-165)
- Polymer-based Optofluidic devices in microchannels fabricated by femtosecond laser irradiation and chemical etching (FLICE). 2009 3rd ICTON Mediterranean Winter Conference (ICTON-MW), 10 December 2009 - 12 December 2009.
- Ultrafast confocal microscope for time-resolved imaging of thin films. CLEO/Europe - EQEC 2009 - European Conference on Lasers and Electro-Optics and the European Quantum Electronics Conference, 14 June 2009 - 19 June 2009.
- Microfluidic channels fabricated by femtosecond laser irradiation and chemical etching for optofluidic devices.. CLEO/Europe - EQEC 2009 - European Conference on Lasers and Electro-Optics and the European Quantum Electronics Conference, 14 June 2009 - 19 June 2009.
- Ultrafast Confocal Microscope for Functional Imaging of Organic Thin Films. Conference on Lasers and Electro-Optics/International Quantum Electronics Conference, 2009.
- Ultrafast confocal microscope for time-resolved imaging of thin films. Optics InfoBase Conference Papers
- Microfluidic channels fabricated by femtosecond laser irradiation and chemical etching for optofluidic devices. Optics InfoBase Conference Papers
- Organic optofluidic devices produced by femtosecond laser micromachining. ISOT: 2009 INTERNATIONAL SYMPOSIUM ON OPTOMECHATRONIC TECHNOLOGIES (pp 404-408)
- Polyfluorene-PMMA copolymers for plastic optical fibers with gain. Organic Optoelectronics and Photonics III
- Ultrafast Photonics in Polymers. Frontiers in Optics 2008/Laser Science XXIV/Plasmonics and Metamaterials/Optical Fabrication and Testing, 2008.
- Ultrafast photonics in polymers. Optics InfoBase Conference Papers
- Ultrafast resonant optical switching in organic materials doped in matrix. Materials Research Society Symposium Proceedings, Vol. 1003 (pp 142-146)
- Nanoscale Imaging of the Interface Dynamics in Polymer Blends by Femtosecond Pump-Probe Confocal Microscopy. Advanced Materials, Vol. 22(28) (pp 3048-3051)
Preprints
- Twisted carotenoids do not support efficient intramolecular singlet fission in the orange carotenoid protein, arXiv.
- Band-edge Excitation of Carotenoids Removes S* Revealing Triplet-pair Contributions to the S1 Absorption Spectrum.
- Manipulating matter with strong coupling: harvesting triplet excitons in organic exciton microcavities, arXiv.
- Spin statistics for triplet-triplet annihilation upconversion: exchange coupling, intermolecular orientation and reverse intersystem crossing, American Chemical Society (ACS).
- Research group
- Research highlights
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In organic solar cells, absorption of light typically creates a tightly bound electron-hole pair. To collect the charges and produce current, the e-h pair must separate.
This happens at a junction between an electron accepting and an electron donating material. By directly tracking the separation of the charges, we showed that they separate to 4nm within 40fs thereby overcoming the electronic Coulomb potential between the electron and hole.
This fast separation occurs due to the wavelike nature of electrons which are governed by fundamental laws of quantum mechanics.
We were able to track the electron-hole separation using the electric field generated between them as they separate.
This electric field perturbs the spectra of the surrounding material and leads to an electro-absorption feature.
Measuring the evolution of the electroabsorption using transient absorption spectroscopy allowed us to track the charge separation in a polymer: PCBM blend and a small molecule: PCBM blend.
A single photon can alter the shape of a molecule. In the eye for example, a photon drives the cis-trans isomerisation which allows us to see.
Using a pump-push-probe technique, we showed that quantum effects can play an important role in this change leading to conformation relaxation rates hundreds of times faster than previously expected.
In general, conformational change occurs on a timescale defined by the energy of the main vibrational mode and the rate of energy dissipation.
Typically, for a conformational change such as a twist around the backbone of a conjugated molecule, this occurs on the tens of picoseconds timescale. However, we demonstrated experimentally that in certain circumstances the molecule, in this case an oligofluorene, can change conformation over two orders of magnitude faster (that is sub-100 fs) in a manner analogous to inertial solvent reorganization demonstrated in the 1990s.
Theoretical simulations demonstrate that non-adiabatic transitions during internal conversion can efficiently convert electronic potential energy into torsional kinetic energy, providing the ‘kick’ that prompts sub-100 fs torsional reorganization.
See news and views of Prof. Mukamel
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Ultrafast triplet formation: two for the price of one [3,4]
In general, photoexcitation leads to an excited state with spin-0 character known as a singlet exciton.
This can convert to a spin-1 excited state (a triplet exciton) through intersystem crossing. In systems made up entirely of Carbon, Nitrogen, Oxygen, Hydrogen or even Sulphur, intersystem crossing generally takes 10s of nanoseconds or more.
However, in certain systems, when the triplet energy is roughly half the singlet energy or less and there is enough space, the singlet can split into two triplet excitons.
The splitting process is known as singlet exciton fission. The ability to generate two excited states from one photon could be used in solar cells to dramatically improve their efficiency.
The fission process is still not fully understood. We have studied a range of materials with the aim of understanding - and one day hopefully controlling - singlet exciton fission.
In polycrystalline pentacene films, singlet fission occurs with a 80fs time-constant [3].
In a polymer poly(3-thienylene-vinylene), it has a time-constant of roughly 45fs [4] and in carotenoid aggregates it ranges from 50-100fs depending on aggregate type [5].
Under intense laser excitation, thin films and suspensions of graphite and its nanostructure, including carbon black, nanotubes, few-layer graphenes and graphene oxides, exhibit induced transparency due to saturable absorption.
This switches to optical limiting only at very high fluences when induced breakdown gives rise to microbubbles and microplasmas that causes nonlinear scattering.
Here, we showed that dispersed graphenes, in contrast, can exhibit broadband nonlinear optical absorption at fluences well below this damage threshold with a strong matrix effect.
We obtained, for nanosecond visible and near-infrared pulses, a new benchmark for optical energy-limiting onset of 10 mJ cm−2 for a linear transmittance of 70%, with excellent output clamping in both heavy-atom solvents and polymer film matrices.
Nanosecond pump–probe spectroscopy in chlorobenzene reveals that the nanographene domains switch from the usual broadband photo-induced bleaching to a novel reverse saturable absorption mechanism with increasing excitation densities across this threshold.
Strong solvent/matrix effect on the nonlinear optical properties of dispersed sub-GOx. a, Plot of output versus input fluence for a neat film of sub-GOx (T'=0.97), and sub-GOx in PMMA (T'=0.40) and in PC (T'=0.055). T ′ is the limiting differential transmittance.
The linear transmittance T is 0.73 for all films. b, Plot of output versus input fluence for sub-GOx dispersed in different solvents compared with C60 in TOL and single-walled CNT in THF, all in cells with 1.0 mm path length. NMP, N-methylpyrrolidinone; THF, tetrahydrofuran; ANS, anisole; MES, mesitylene; DFB, 1,3-difluorobenzene;
BN, benzonitrile; CB, chlorobenzene; BB, bromobenzene; DCB, 1,2-dichlorobenzene; TCB, 1,2,4-trichlorobenzene; TOL, toluene. T is 0.70.The large non-linear effect is due to the formation of localised exciton-like states which we attribute to triplet excitons due to the heavy-atom effect.
We speculate that the initial electron–hole gas condenses to triplet-like excitons when promoted by spin–orbit coupling with heavy atoms.
In contrast, in graphite or multilayer graphenes in which the inner layers are effectively isolated from the environment, the electron–hole gas cools and recombines rapidly.
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Ultrafast all-optical switching in plastic optical fibers [7]
The ability to switch light with sub-picosecond time-scales in an optical fiber network is important for improved signal data communication speed and potentially for optical computing.
We made a logical NOT gate using gain switching in isolated conjugated fluorene oligomers. We use the fact that charge absorption overlaps with stimulated emission and generate charges on the oligomers which recombine within a few tens of femtoseconds.
The change from amplification through stimulated emission to loss through charge absorption produces a large switching signal and the recombination allows for ultrafast sub 100fs switching.
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