Lukasz Piatkowski

Generation of photovoltage in graphene on a femtosecond timescale through efficient carrier heating

Graphene is a promising material for ultrafast and broadband photodetection. Earlier studies have addressed the general operation of graphene-based photothermoelectric devices and the switching speed, which is limited by the charge carrier cooling time, on the order of picoseconds. However, the generation of the photovoltage could occur at a much faster timescale, as it is associated with the carrier heating time. Here, we measure the photovoltage generation time and find it to be faster than 50 fs. As a proof-of-principle application of this ultrafast photodetector, we use graphene to directly measure, electrically, the pulse duration of a sub-50 fs laser pulse. The observation that carrier heating is ultrafast suggests that energy from absorbed photons can be efficiently transferred to carrier heat. To study this, we examine the spectral response and find a constant spectral responsivity of between 500 and 1,500 nm. This is consistent with efficient electron heating. These results are promising for ultrafast femtosecond and broadband photodetector applications.

Capturing the Optical Phase Response of Nanoantennas by Coherent Second-Harmonic Microscopy

The ultrafast coherent control of light localization in resonant plasmonic nanostructures is intricately related to the phase response of the involved plasmon resonances. In this work, we exploit the second harmonic signal generated by single optical nanoantennas subject to broadband phase-controlled femtosecond pulses to study and tailor the coherent resonance response. Our results reveal that both the spectral phase and the amplitude components associated with the plasmon resonance of arbitrary individual nanoantennas can be accurately determined.

Hot-carrier photocurrent effects at graphene–metal interfaces

Photoexcitation of graphene leads to an interesting sequence of phenomena, some of which can be exploited in optoelectronic devices based on graphene. In particular, the efficient and ultrafast generation of an electron distribution with an elevated electron temperature and the concomitant generation of a photo-thermoelectric voltage at symmetry-breaking interfaces is of interest for photosensing and light harvesting. Here, we experimentally study the generated photocurrent at the graphene-metal interface, focusing on the time-resolved photocurrent, the effects of photon energy, Fermi energy and light polarization. We show that a single framework based on photo-thermoelectric photocurrent generation explains all experimental results.

Broadband single-molecule excitation spectroscopy

Over the past 25 years, single-molecule spectroscopy has developed into a widely used tool in multiple disciplines of science. The diversity of routinely recorded emission spectra does underpin the strength of the single-molecule approach in resolving the heterogeneity and dynamics, otherwise hidden in the ensemble. In early cryogenic studies single molecules were identified by their distinct excitation spectra, yet measuring excitation spectra at room temperature remains challenging. Here we present a broadband Fourier approach that allows rapid recording of excitation spectra of individual molecules under ambient conditions and that is robust against blinking and bleaching. Applying the method we show that the excitation spectra of individual molecules exhibit an extreme distribution of solvatochromic shifts and distinct spectral shapes. Importantly, we demonstrate that the sensitivity and speed of the broadband technique is comparable to that of emission spectroscopy putting both techniques side-by-side in single-molecule spectroscopy.

Nature of Large Temporal Fluctuations of Hydrogen Transfer Rates in Single Molecules

Double hydrogen transfer was monitored in single molecules of parent porphycene and its tetra- t-butyl derivative using confocal fluorescence microscopy. The molecules have been embedded in a polymer matrix. Under such conditions, a significant fraction of the population reveals a huge decrease of the tautomerization rate with respect to the value obtained from ensemble studies in solution. This effect is explained by a model that assumes that the rate is determined by the reorganization coordinate that involves slow relaxation of the polymer matrix. The model provides indirect evidence for the dominant role of tunneling. It is proposed that tautomerization in single molecules of the porphycene family can be used to probe polymer relaxation dynamics on the time scale ranging from picoseconds to minutes.

Resonant plasmonic nanoparticles for multicolor second harmonic imaging

Nanoparticles capable of efficiently generating nonlinear optical signals, like second harmonic generation, are attracting a lot of attention as potential background-free and stable nano-probes for biological imaging. However, second harmonic nanoparticles of different species do not produce readily distinguishable optical signals, as the excitation laser mainly defines their second harmonic spectrum. This is in marked contrast to other fluorescent nano-probes like quantum dots that emit light at different colors depending on their sizes and materials. Here, we present the use of resonant plasmonic nanoparticles, combined with broadband phase-controlled laser pulses, as tunable sources of multicolor second harmonic generation. The resonant plasmonic nanoparticles strongly interact with the electromagnetic field of the incident light, enhancing the efficiency of nonlinear optical processes. Because the plasmon resonance in these structures is spectrally narrower than the laser bandwidth, the plasmonic nanoparticles imprint their fingerprints on the second harmonic spectrum. We show how nanoparticles of different sizes produce different colors in the second harmonic spectra even when excited with the same laser pulse. Using these resonant plasmonic nanoparticles as nano-probes is promising for multicolor second harmonic imaging while keeping all the advantages of nonlinear optical microscopy.

Ultrafast Stimulated Emission Nanoscopy for Charge Dynamics, fs-Detection and Nanolasing

We present a newly developed technique called time-resolved stimulated emission nanoscopy, which enables imaging and studying the femtosecond dynamics in nanosamples. Direct insights into femtosecond charge transfer and relaxation pathways in semiconductor nanoparticles are presented.