Giulio Cerullo

Giulio Cerullo
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Giulio Cerullo
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Physics - Materials Science (6)
 
Physics - Mesoscopic Systems and Quantum Hall Effect (6)
 
Physics - Optics (5)
 
Physics - Strongly Correlated Electrons (2)
 
Physics - Biological Physics (1)
 
Physics - Superconductivity (1)
 
Physics - Chemical Physics (1)
 
Physics - Soft Condensed Matter (1)
 
Quantum Physics (1)

Publications Authored By Giulio Cerullo

Electronic properties and lattice vibrations are supposed to be strongly correlated in metal-halide perovskites, due to the "soft" fluctuating nature of their crystal lattice. Thus, unveiling electron-phonon coupling dynamics upon ultra-fast photoexcitation is necessary for understanding the optoelectronic behaviour of the semiconductor. Here, we use impulsive vibrational spectroscopy to reveal ground and excited state vibrational modes of methylammonium lead-bromide perovskite. Read More

Transition metal dichalcogenides (TMDs) are emerging as promising two-dimensional (2d) semiconductors for optoelectronic and flexible devices. However, a microscopic explanation of their photophysics -- of pivotal importance for the understanding and optimization of device operation -- is still lacking. Here we use femtosecond transient absorption spectroscopy, with pump pulse tunability and broadband probing, to monitor the relaxation dynamics of single-layer MoS2 over the entire visible range, upon photoexcitation of different excitonic transitions. Read More

In band-like semiconductors, charge carriers form a thermal energy distribution rapidly after optical excitation. In hybrid lead halide perovskites, the cooling of such thermal distributions has been reported to occur on timescales of ~300 fs via carrier-phonon scattering. However, the initial step of build-up of a thermal Boltzmann distribution proved difficult to resolve with conventional pump-probe techniques due to the requirement of high resolution both in time and in energy. Read More

Organic semiconductors have the remarkable property that their optical excitation not only generates charge-neutral electron-hole pairs (excitons) but also charge-separated polaron pairs with high yield. The microscopic mechanisms underlying this charge separation have been debated for many years. Here we use ultrafast two-dimensional electronic spectroscopy to study the dynamics of polaron pair formation in a prototypical polymer thin film on a sub-20-fs time scale. Read More

The calculation of the equilibrium optical properties of bulk silicon by using the Bethe--Salpeter equation solved in the Kohn--Sham basis represents a cornerstone in the development of an ab--initio approach to the optical and electronic properties of materials. Nevertheless calculations of the {\em transient} optical spectrum using the same efficient and successful scheme are scarce. We report, here, a joint theoretical and experimental study of the transient reflectivity spectrum of bulk silicon. Read More

We study how the color and polarization of ultrashort pulses of visible light can be used to control the demagnetization processes of the antiferromagnetic insulator Cr$_2$O$_3$. We utilize time-resolved second harmonic generation (SHG) to probe how changes in the magnetic and structural state evolve in time. We show that, varying the pump photon-energy to excite either localized transitions within the Cr or charge transfer states, leads to markedly different dynamics. Read More

An intrinsic instability towards inhomogeneous states is emerging as the prominent feature of underdoped cuprates and manifests itself in a variety of ways including the spontaneous emergence of charge-order patterns at low temperature. The experimental evidences show a general trend where various instabilities, that break different symmetries at the nanometric scale, appear below a characteristic temperature and only up to a critical hole doping p$_{cr}$. This revives the long debated question whether this behaviour is just the consequence of the tendency to develop a specific long-range symmetry-broken phase, or it is the low-energy manifestation of a more general precursory state, which arises from strong electronic correlations suddenly changing at p$_{cr}$. Read More

The two-dimensional semiconductor MoS2 in its mono- and few-layer form is expected to have a significant exciton binding energy of several 100 meV, leading to the consensus that excitons are the primary photoexcited species. Nevertheless, even single layers show a strong photovoltaic effect and work as the active material in high sensitivity photodetectors, thus indicating efficient charge carrier photogeneration (CPG). Here we use continuous wave photomodulation spectroscopy to identify the optical signature of long-lived charge carriers and femtosecond pump-probe spectroscopy to follow the CPG dynamics. Read More

Boosting nonlinear frequency conversion in extremely confined volumes remains a key challenge in nano-optics, nanomedicine, photocatalysis, and background-free biosensing. To this aim, field enhancements in plasmonic nanostructures are often exploited to effectively compensate for the lack of phase-matching at the nanoscale. Second harmonic generation (SHG) is, however, strongly quenched by the high degree of symmetry in plasmonic materials at the atomic scale and in nanoantenna designs. Read More

Theory predicts peculiar features for excited-state dynamics in one dimension (1D) that are difficult to be observed experimentally. Single-walled carbon nanotubes (SWNTs) are an excellent approximation to 1D quantum confinement, due to their very high aspect ratio and low density of defects. Here we use ultrafast optical spectroscopy to probe photogenerated charge-carriers in (6,5) semiconducting SWNTs. Read More

The non-equilibrium semiconductors physics is based on the paradigm that different degrees of freedom interact on different timescales. In this context the photo-excitation is often treated as an impulsive injection of electronic energy that is transferred to other degrees of freedom only at later times. Here, by studying the ultrafast particles dynamics in a archetypal strongly correlated charge-transfer insulator (La2CuO4), we show that the interaction between electrons and bosons manifest itself directly in the photo-excitation processes of a correlated material. Read More

We present a combined analytical and numerical study of the early stages (sub-100fs) of the non-equilibrium dynamics of photo-excited electrons in graphene. We employ the semiclassical Boltzmann equation with a collision integral that includes contributions from electron-electron (e-e) and electron-optical phonon interactions. Taking advantage of circular symmetry and employing the massless Dirac Fermion (MDF) Hamiltonian, we are able to perform an essentially analytical study of the e-e contribution to the collision integral. Read More

Sharp metallic nanotapers irradiated with few-cycle laser pulses are emerging as a source of highly confined coherent electron wavepackets with attosecond duration and strong directivity. The possibility to steer, control or switch such electron wavepackets by light is expected to pave the way towards direct visualization of nanoplasmonic field dynamics and real-time probing of electron motion in solid state nanostructures. Such pulses can be generated by strong-field induced tunneling and acceleration of electrons in the near-field of sharp gold tapers within one half-cycle of the driving laser field. Read More

The coherent dynamics of vibronic wave packets in the green fluorescent protein is reported. At room temperature the non-stationary dynamics following impulsive photoexcitation displays an oscillating optical transmissivity pattern with components at 67 fs (497 cm-1) and 59 fs (593 cm-1). Our results are complemented by ab initio calculations of the vibrational spectrum of the chromophore. Read More