Ultrafast optical techniques provide powerful probes of different states of matter, using light pulses that have femtosecond duration. In Warwick our activities span a number of areas:
studying the dynamics of the light-matter interaction in novel compounds and nanomaterials via terahertz spectroscopy and pump-probe methods,
performing terahertz medical imaging and spectroscopy,
developing methods and components for terahertz imaging and terahertz spectroscopy.
Group facilities
The Group has labs across the campus, in the main Physics building, Materials and Analytical Sciences, and Millburn House. Read more about our experimental capabilities in terahertz science and technology. We also run the Warwick Centre for Ultrafast Spectroscopy Research Technology Platform.
Please get in touch if you are interested in a PhD or MSc by Research in the group. We are also happy to support postdoctoral researchers to apply for fellowship schemes.
We use pump/probe spectroscopy to study how light and matter interact on femtosecond to nanosecond timescales. Using visible probes we can track electronic processes, while infrared radiation lets us study vibrational states of molecules and atomic-scale defects in semiconductors.
Performing in vivo studies of the THz properties of skin is a major initiative in the group, supported by the EPSRC Terabotics Programme GrantLink opens in a new window. We develop robust measurement protocols and test them on a statistically significant number of patients, cross-checking with other methods.
A major strand of our research is to improve our knowledge of the fundamental science underpinning new semiconductor materials, such as metal-halide perovskites, which are often attractive for photovoltaic applications.
We develop new THz devices and integrate them into novel systems designs that can perform THz imaging and THz spectroscopy faster, and with increased capabilities (e.g. polarisation control; robot-controlled probes).
T.J. Keat, D. J. L. Coxon, R.J. Cruddace, V. G. Stavros, M. E. Newton, and J. Lloyd-Hughes Diamond and Related Materials 141110661 (Jan 2024)
The dynamics of the 3237 cm−1 local vibrational mode in diamond, associated with an unknown defect, was investigated using ultrafast infrared pump-probe spectroscopy. When pumped at 3237 cm−1, a degenerate probe was used to study the ground state's recovery, while a non-degenerate probe tracked excited state absorption at 3029 cm−1, corresponding to the 1 → 2 vibrational state transition. The similar population lifetimes for the ground state recovery and excited state absorption suggests a single population decay pathway, with a lifetime of T1=2.2+-0.1ps. Perturbed free induction decay signals observed in negative time delays gave the dephasing time of the coherent state between the 0 and 1 vibrational states, and further predicted the 3029 cm−1 transition. Images from FTIR microscopy show that the 3237 cm−1 feature and the 3107 cm−1 absorption line from the N3VH0 defect are not correlated, and our pump-probe study shows the 3237 cm−1 feature does not share a common ground state with the N3VH0 defect, both of which suggest that this local vibrational mode does not originate from the N3VH0 defect. A calibration factor was obtained via a Morse potential model constrained by the observed transition energies, which relates the concentration of the defect producing the 3237 cm−1 feature to its absorption coefficient measured by FTIR spectroscopy. Based on FTIR absorption spectroscopy under uniaxial stress, we further assign a trigonal symmetry character to the defect that gives the 3237 cm−1 feature. The results presented are consistent with the theory that the 3237 cm−1 feature originates from the N4VH defect, the quantification of which allows better tracking of the nitrogen content in diamond.
Nathaniel P. Gallop, Dumitru Sirbu, David Walker, James Lloyd-Hughes, Pablo Docampo and Rebecca L. Milot ACS Photonics 104022, (October 2023)
We report on the emission of high-intensity pulsed terahertz radiation from the metal-free halide perovskite single crystal methyl-DABCO ammonium iodide (MDNI) under femtosecond illumination. The power and angular dependence of the THz output implicate optical rectification of the 800 nm pump as the mechanism of THz generation. Further characterization finds that, for certain crystal orientations, the angular dependence of THz emission is modulated by phonon resonances attributable to the motion of the methyl-DABCO moiety. At maximum, the THz emission spectrum of MDNI is free from significant phonon resonances, resulting in THz pulses with a temporal width of <900 fs and a peak-to-peak electric field strength of approximately 0.8 kV cm–1─2 orders of magnitude higher than any other reported halide perovskite emitters. Our results point toward metal-free perovskites as a promising new class of THz emitters that brings to bear many of the advantages enjoyed by other halide perovskite materials. In particular, the broad tunability of optoelectronic properties and ease of fabrication of perovskite materials opens up the possibility of further optimizing the THz emission properties within this material class.
A. Ren, H. Wang, L. Dai, J. Xia, E. Butler-Caddle, J.A. Smith, ... S.A. Hindmarsh, A.M. Sanchez, J. Lloyd-Hughes, S. J Sweeney, ... and Wei Zhang Nature Photonics17, 798–805 (July 2023)
Light-emitting diodes (LEDs) are ubiquitous in modern society, with applications spanning from lighting and displays to medical diagnostics and data communications. Metal-halide perovskites are promising materials for LEDs because of their excellent optoelectronic properties and solution processability. Although research has progressed substantially in optimizing their external quantum efficiency, the modulation characteristics of perovskite LEDs remain unclear. Here we report a holistic approach for realizing fast perovskite photonic sources on silicon based on tailoring alkylammonium cations in perovskite systems. We reveal the recombination behaviour of charged species at various carrier density regimes relevant for their modulation performance. By integrating a Fabry–Pérot microcavity on silicon, we demonstrate perovskite devices with efficient light outcoupling. We achieve device modulation bandwidths of up to 42.6 MHz and data rates above 50 Mbps, with further analysis suggesting that the bandwidth may exceed gigahertz levels. The principles developed here will support the development of perovskite light sources for next-generation data-communication architectures. The demonstration of solution-processed perovskite emitters on silicon substrates also opens up the possibility of integration with micro-electronics platforms.
Jake D. Hutchinson, Edoardo Ruggeri, Jack M. Woolley, Géraud Delport, Samuel D. Stranks, Rebecca L. Milot Advanced Functional Materials2305736, (August 2023)
Mixed 2D/3D perovskite materials are of particular interest to the photovoltaics and light- emitting diode (LED) communities due to their impressive opto-electronic properties alongside improved moisture stability compared to conventional 3D perovskite absorbers. Here, a mixed lead-tin perovskite containing distinct, self-assembled domains of either 3D structures or highly phase-pure Ruddlesden–Popper 2D structures is studied. The complex energy landscape of the material is revealed with ultrafast optical transient absorption measurements. It is shown that charge transfer between these microscale domains only occurs on nanosecond timescales, consistent with the large size of the domains. Using optical pump-terahertz probe spectroscopy, the effective charge-carrier mobility is shown to be an intermediary between analogous pure 2D and 3D perovskites. Furthermore, detailed analysis of the free carrier recombination dynamics is presented. By combining results from a range of excitation wavelengths within a full dynamic model of the photoexcited carrier population, it is shown that the 2D domains in the film exhibit remarkably similar carrier dynamics to the 3D domains, suggesting that long-range charge-transport should not be impeded by the heterogeneous structure of the material.