In the 60 years since the invention of the laser, the scientific community has developed numerous fields of research based on these bright, coherent light sources, including the areas of imaging, spectroscopy, materials processing and communications. Ultrafast spectroscopy and imaging techniques are at the forefront of research into the light–matter interaction at the shortest times accessible to experiments, ranging from a few attoseconds to nanoseconds. Light pulses provide a crucial probe of the dynamical motion of charges, spins, and atoms on picosecond, femtosecond, and down to attosecond timescales, none of which are accessible even with the fastest electronic devices. Furthermore, strong light pulses can drive materials into unusual phases, with exotic properties. In this roadmap we describe the current state-of-the-art in experimental and theoretical studies of condensed matter using ultrafast probes. In each contribution, the authors also use their extensive knowledge to highlight challenges and predict future trends.

Measuring terahertz (THz) conductivity on an ultrafast timescale is an excellent way to observe charge-carrier dynamics in semiconductors as a function of time after photoexcitation. However, a conductivity measurement alone cannot separate the effects of charge-carrier recombination from effective mass changes as charges cool and experience different regions of the electronic band structure. Here we present a form of time-resolved magneto-THz spectroscopy that allows us to measure cyclotron effective mass on a picosecond timescale. We demonstrate this technique by observing electron cooling in the technologically significant narrow-bandgap semiconductor indium antimonide. A significant reduction of electron effective mass from 0.032 to 0.017 me is observed in the first 200 ps after injecting hot electrons. The measured electron effective mass in InSb as a function of photoinjected electron density agrees well with conduction band nonparabolicity predictions from ab initio calculations of the quasiparticle band structure.

Layered hybrid perovskites (LPKs) have emerged as a viable solution to address perovskite stability concerns and enable their implementation in wide-scale energy harvesting. Yet, although more stable, the performance of devices incorporating LPKs still lags behind that of state-of-the-art, multi-cation perovskite materials. This is typically assigned to their poor charge transport, currently caused by the choice of cations used within the organic layer. On balance, a compromise between efficiency and stability is sought, involving careful control of phase purity and distribution, interfaces and energy/charge transfer processes. Further progress is hindered by the difficulty in identifying the fundamental optoelectronic processes in these materials. Here, the high exciton binding energy of LPKs lead to the formation of multiple photoexcited species, which greatly complicate measurement interpretation. In this light, this review gives an overview of how complementary measurement techniques must be used to separate the contributions from the different species in order to identify device bottlenecks, and become a useful tool to narrow down the limitless list of organic cations. A move away from making compromises to mitigate the impact of poor charge transport is required. The root of the problem must be addressed instead through rational design of the interlayer cations.

The development of THz technology and communication systems is creating demand for devices that can modulate THz beams rapidly. Here we report the design and characterisation of high-performance, broadband THz modulators based on the photo-induced transparency of carbon nanotube films. Rather than operating in the standard modulation mode, where optical excitation lowers transmission, this new class of modulators exhibits an inverted modulation mode with an enhanced transmission. Under femtosecond pulsed illumination, modulation depths reaching +80% were obtained simultaneously with modulation speeds of 340 GHz. The influence of the film thickness on the insertion loss, modulation speed and modulation depth was explored over a frequency range from 400 GHz to 2.6 THz. The excellent modulation depth and high modulation speed demonstrated the significant potential of carbon nanotube thin films for ultrafast THz modulators.