arXiv subjects

Andrea Cavalleri

Publications and source records attributed to Andrea Cavalleri.

At least 55 records · Page 3Linked to original sources

arXiv2017

Transiently enhanced interlayer tunneling in optically driven high $T_c$ superconductors

Recent pump-probe experiments reported an enhancement of superconducting transport along the $c$-axis of underdoped YBa$_2$Cu$_3$O$_{6+δ}$ (YBCO), induced by a mid-infrared optical pump pulse tuned to a specific lattice vibration. To understand this transient non-equilibrium state, we develop a pump-probe formalism for a stack of Josephson junctions, and we consider the tunneling strengths in presence of modulation with an ultrashort optical pulse. We demonstrate that a transient enhancement of the Josephson coupling can be obtained for pulsed excitation and that this can be even larger than in a continuously driven steady-state. Especially interesting is the conclusion that the effect is largest when the material is parametrically driven at a frequency immediately above the plasma frequency, in agreement with what is found experimentally. For bilayer Josephson junctions, an enhancement similar to that experimentally is predicted below the critical temperature $T_c$. This model reproduces the essential features of the enhancement measured below $T_c$. To reproduce the experimental results above $T_c$, we will explore extensions of this model, such as in-plane and amplitude fluctuations, elsewhere.

cond-mat.supr-con↗

arXiv2017

Parametric amplification of optical phonons

Amplification of light through stimulated emission or nonlinear optical interactions has had a transformative impact on modern science and technology. The amplification of other bosonic excitations, like phonons in solids, is likely to open up new remarkable physical phenomena. Here, we report on an experimental demonstration of optical phonon amplification. A coherent mid-infrared optical field is used to drive large amplitude oscillations of the Si-C stretching mode in silicon carbide. Upon nonlinear phonon excitation, a second probe pulse experiences parametric optical gain at all wavelengths throughout the reststrahlen band, which reflects the amplification of optical-phonon fluctuations. Starting from first principle calculations, we show that the high-frequency dielectric permittivity and the phonon oscillator strength depend quadratically on the lattice coordinate. In the experimental conditions explored here, these oscillate then at twice the frequency of the optical field and provide a parametric drive for lattice fluctuations. Parametric gain in phononic four wave mixing is a generic mechanism that can be extended to all polar modes of solids, as a new means to control the kinetics of phase transitions, to amplify many body interactions or to control phonon-polariton waves.

cond-mat.mtrl-sci↗

arXiv2017

Probing the Interatomic Potential of Solids by Strong-Field Nonlinear Phononics

Femtosecond optical pulses at mid-infrared frequencies have opened up the nonlinear control of lattice vibrations in solids. So far, all applications have relied on second order phonon nonlinearities, which are dominant at field strengths near 1 MVcm-1. In this regime, nonlinear phononics can transiently change the average lattice structure, and with it the functionality of a material. Here, we achieve an order-of-magnitude increase in field strength, and explore higher-order lattice nonlinearities. We drive up to five phonon harmonics of the A1 mode in LiNbO3. Phase-sensitive measurements of atomic trajectories in this regime are used to experimentally reconstruct the interatomic potential and to benchmark ab-initio calculations for this material. Tomography of the Free Energy surface by high-order nonlinear phononics will impact many aspects of materials research, including the study of classical and quantum phase transitions.

cond-mat.mtrl-sci↗

arXiv2017

Terahertz field control of interlayer transport modes in cuprate superconductors

We theoretically show that terahertz pulses with controlled amplitude and frequency can be used to switch between stable transport modes in layered superconductors, modelled as stacks of Josephson junctions. We find pulse shapes that deterministically switch the transport mode between superconducting, resistive and solitonic states. We develop a simple model that explains the switching mechanism as a destablization of the centre of mass excitation of the Josephson phase, made possible by the highly non-linear nature of the light-matter coupling.

cond-mat.supr-con↗

arXiv2017

Theory of enhanced interlayer tunneling in optically driven high $T_c$ superconductors

Motivated by recent pump-probe experiments indicating enhanced coherent $c$-axis transport in underdoped YBCO, we study Josephson junctions periodically driven by optical pulses. We propose a mechanism for this observation by demonstrating that a parametrically driven Josephson junction shows an enhanced imaginary part of the low-frequency conductivity when the driving frequency is above the plasma frequency, implying an effectively enhanced Josephson coupling. We generalize this analysis to a bilayer system of Josephson junctions modeling YBCO. Again, the Josephson coupling is enhanced when the pump frequency is blue-detuned to either of the two plasma frequencies of the material. We show that the emergent driven state is a genuine, non-equilibrium superconducting state, in which equilibrium relations between the Josephson coupling, current fluctuations, and the critical current no longer hold.

cond-mat.supr-con↗

arXiv2017

Ultrafast reversal of the ferroelectric polarization

The ability to manipulate ferroelectrics at ultrafast speeds has long been an elusive target for materials research. Coherently exciting the ferroelectric mode with ultrashort optical pulses holds the promise to switch the ferroelectric polarization on femtosecond timescale, two orders of magnitude faster compared to what is possible today with pulsed electric fields. Here, we report on the demonstration of ultrafast optical reversal of the ferroelectric polarization in LiNbO3. Rather than driving the ferroelectric mode directly, we couple to it indirectly by resonant excitation of an auxiliary high-frequency phonon mode with femtosecond mid-infrared pulses. Due to strong anharmonic coupling between these modes, the atoms are directionally displaced along the ferroelectric mode and the polarization is transiently reversed, as revealed by time-resolved, phase-sensitive second-harmonic generation. This reversal can be induced in both directions, a key pre-requisite for practical applications.

cond-mat.mtrl-sci↗

arXiv2017

A dynamical stability limit for the charge density wave in K0.3MoO3

We study the response of the one-dimensional charge density wave in K0.3MoO3 to different types of excitation with femtosecond optical pulses. We compare the response to direct excitation of the lattice at mid-infrared frequencies with that to the injection of quasi-particles across the low-energy charge density wave gap and to charge transfer excitations in the near infrared. For all three cases, we observe a fluence threshold above which the amplitude-mode oscillation frequency is softened and the mode becomes increasingly damped. We show that all the data can be collapsed onto a universal curve in which the melting of the charge density wave occurs abruptly at a critical lattice excursion. These data highlight the existence of a universal stability limit for a charge density wave, reminiscent of the empirical Lindemann criterion for the stability of a crystal lattice.

cond-mat.str-el↗

arXiv2016

Nonlinear light-matter interaction at terahertz frequencies

Strong optical pulses at mid-infrared and terahertz frequencies have recently emerged as a powerful tool to manipulate and control the solid state and especially complex condensed matter systems with strongly correlated electrons. The recent developments in high-power sources in the 0.1-30 THz frequency range, both from table-top laser systems and Free-Electron Lasers, has provided access to excitations of molecules and solids, which can be stimulated at their resonance frequencies. Amongst these, we discuss free electrons in metals, superconducting gaps and Josephson plasmons in layered superconductors, vibrational modes of the crystal lattice (phonons), as well as magnetic excitations. This Review provides an overview and illustrative examples of how intense THz transients can be used to resonantly control matter, with particular focus on strongly correlated electron systems and high-temperature superconductors.

cond-mat.str-el↗

arXiv2016

Electronic-structural Dynamics in Graphene

We review our recent time- and angle-resolved photoemission spectroscopy experiments, which measure the transient electronic structure of optically driven graphene. For pump photon energies in the near infrared ($\hbarω_{\text{pump}}=950$meV) we have discovered the formation of a population-inverted state near the Dirac point, which may be of interest for the design of THz lasing devices and optical amplifiers. At lower pump photon energies ($\hbarω_{\text{pump}}<400$meV), for which interband absorption is not possible in doped samples, we find evidence for free carrier absorption. In addition, when mid-infrared pulses are made resonant with an infrared-active in-plane phonon of bilayer graphene ($\hbarω_{\text{pump}}=200$meV), a transient enhancement of the electron-phonon coupling constant is observed, providing interesting perspective for experiments that report light-enhanced superconductivity in doped fullerites in which a similar lattice mode was excited. All the studies reviewed here have important implications for applications of graphene in optoelectronic devices and for the dynamical engineering of electronic properties with light.

cond-mat.mtrl-sci↗

arXiv2016

Proposed cavity Josephson plasmonics with complex-oxide heterostructures

We discuss how complex-oxide heterostructures that include high-Tc superconducting cuprates can be used to realize an array of sub-millimeter cavities that support Josephson plasmon polaritons. These cavities have several attractive features for new types of light matter interaction studies and we show that they promote "ultrastrong" coupling between THz frequency radiation and Josephson plasmons. Cavity electrodynamics of Josephson plasmons allows to manipulate the superconducting order-parameter phase coherence. As an example, we discuss how it could be used to cool superconducting phase fluctuations with light.

cond-mat.supr-con↗

arXiv2015

Parametric Amplification of a Terahertz Quantum Plasma Wave

Many applications in photonics require all-optical manipulation of plasma waves, which can concentrate electromagnetic energy on sub-wavelength length scales. This is difficult in metallic plasmas because of their small optical nonlinearities. Some layered superconductors support weakly damped plasma waves, involving oscillatory tunneling of the superfluid between capacitively coupled planes. Such Josephson plasma waves (JPWs) are also highly nonlinear, and exhibit striking phenomena like cooperative emission of coherent terahertz radiation, superconductor-metal oscillations and soliton formation. We show here that terahertz JPWs in cuprate superconductors can be parametrically amplified through the cubic tunneling nonlinearity. Parametric amplification is sensitive to the relative phase between pump and seed waves and may be optimized to achieve squeezing of the order parameter phase fluctuations or single terahertz-photon devices.

cond-mat.supr-con↗

arXiv2014

Phonon-pump XUV-photoemission-probe in graphene: evidence for non-adiabatic heating of Dirac carriers by lattice deformation

We modulate the atomic structure of bilayer graphene by driving its lattice at resonance with the in-plane E1u lattice vibration at 6.3um. Using time- and angle-resolved photoemission spectroscopy (tr-ARPES) with extreme ultra-violet (XUV) pulses, we measure the response of the Dirac electrons near the K-point. We observe that lattice modulation causes anomalous carrier dynamics, with the Dirac electrons reaching lower peak temperatures and relaxing at faster rate compared to when the excitation is applied away from the phonon resonance or in monolayer samples. Frozen phonon calculations predict dramatic band structure changes when the E1u vibration is driven, which we use to explain the anomalous dynamics observed in the experiment.

cond-mat.mes-hall↗

arXiv2014

Population Inversion in Monolayer and Bilayer Graphene

The recent demonstration of saturable absorption and negative optical conductivity in the Terahertz range in graphene has opened up new opportunities for optoelectronic applications based on this and other low dimensional materials. Recently, population inversion across the Dirac point has been observed directly by time- and angle-resolved photoemission spectroscopy (tr-ARPES), revealing a relaxation time of only ~ 130 femtoseconds. This severely limits the applicability of single layer graphene to, for example, Terahertz light amplification. Here we use tr-ARPES to demonstrate long-lived population inversion in bilayer graphene. The effect is attributed to the small band gap found in this compound. We propose a microscopic model for these observations and speculate that an enhancement of both the pump photon energy and the pump fluence may further increase this lifetime.

cond-mat.mtrl-sci↗

arXiv2014

Theory of nonlinear phononics for coherent light-control of solids

We present a microscopic theory for ultrafast control of solids with high-intensity terahertz frequency optical pulses. When resonant with selected infrared-active vibrations, these pulses transiently modify the crystal structure and lead to new collective electronic properties. The theory predicts the dynamical path taken by the crystal lattice using first-principles calculations of the energy surface and classical equations of motion, as well as symmetry considerations. Two classes of dynamics are identified. In the perturbative regime, displacements along the normal mode coordinate of symmetry-preserving Raman active modes can be achieved by cubic anharmonicities. This explains the light-induced insulator-to-metal transition reported experimentally in manganites. We predict a regime in which ultrafast instabilities that break crystal symmetry can be induced. This nonperturbative effect involves a quartic anharmonic coupling and occurs above a critical threshold, below which the nonlinear dynamics of the driven mode displays softening and dynamical stabilization.

cond-mat.str-el↗

arXiv2013

Snapshots of non-equilibrium Dirac carrier distributions in graphene

The optical properties of graphene are made unique by the linear band structure and the vanishing density of states at the Dirac point. It has been proposed that even in the absence of a semiconducting bandgap, a relaxation bottleneck at the Dirac point may allow for population inversion and lasing at arbitrarily long wavelengths. Furthermore, efficient carrier multiplication by impact ionization has been discussed in the context of light harvesting applications. However, all these effects are difficult to test quantitatively by measuring the transient optical properties alone, as these only indirectly reflect the energy and momentum dependent carrier distributions. Here, we use time- and angle-resolved photoemission spectroscopy with femtosecond extreme ultra-violet (EUV) pulses at 31.5 eV photon energy to directly probe the non-equilibrium response of Dirac electrons near the K-point of the Brillouin zone. In lightly hole-doped epitaxial graphene samples, we explore excitation in the mid- and near-infrared, both below and above the minimum photon energy for direct interband transitions. While excitation in the mid-infrared results only in heating of the equilibrium carrier distribution, interband excitations give rise to population inversion, suggesting that terahertz lasing may be possible. However, in neither excitation regime do we find indication for carrier multiplication, questioning the applicability of graphene for light harvesting. Time-resolved photoemission spectroscopy in the EUV emerges as the technique of choice to assess the suitability of new materials for optoelectronics, providing quantitatively accurate measurements of non-equilibrium carriers at all energies and wavevectors.

cond-mat.mes-hall↗

arXiv2011

Nonlinear phononics: A new ultrafast route to lattice control

To date, two types of coupling between electromagnetic radiation and a crystal lattice have been identified experimentally. One is direct, for infrared (IR)-active vibrations that carry an electric dipole. The second is indirect, it occurs through intermediate excitation of the electronic system via electron-phonon coupling, as in stimulated Raman scattering. Nearly 40 years ago, proposals were made of a third path, referred to as ionic Raman scattering (IRS). It was posited that excitation of an IR-active phonon could serve as the intermediate state for a Raman scattering process relying on lattice anharmonicity as opposed to electron phonon interaction. In this paper, we report an experimental demonstration of ionic Raman scattering and show that this mechanism is relevant to optical control in solids. The key insight is that a rectified phonon field can exert a directional force onto the crystal, inducing an abrupt displacement of the atoms from the equilibrium positions that could not be achieved through excitation of an IR-active vibration alone, for which the force is oscillatory. IRS opens up a new direction for the coherent control of solids in their electronic ground state, different from approaches that rely on electronic excitations.

cond-mat.other↗

arXiv2010

Momentum-dependent snapshots of a melting charge density wave

Charge density waves (CDWs) underpin the electronic properties of many complex materials. Near-equilibrium CDW order is linearly coupled to a periodic, atomic-structural distortion, and the dynamics is understood in terms of amplitude and phase modes. However, at the shortest timescales lattice and charge order may become de-coupled, highlighting the electronic nature of this many-body broken symmetry ground state. Using time and angle resolved photoemission spectroscopy with sub-30-fs XUV pulses, we have mapped the time- and momentum-dependent electronic structure in photo-stimulated 1T-TaS2, a prototypical two-dimensional charge density wave compound. We find that CDW order, observed as a splitting of the uppermost electronic bands at the Brillouin zone boundary, melts well before relaxation of the underlying structural distortion. Decoupled charge and lattice modulations challenge the view of Fermi Surface nesting as a driving force for charge density wave formation in 1T-TaS2.

cond-mat.str-el↗

arXiv2010

Polaronic conductivity in the photoinduced phase of 1T-TaS2

The transient optical conductivity of photoexcited 1T-TaS2 is determined over a three-order-of-magnitude frequency range. Prompt collapse and recovery of the Mott gap is observed. However, we find important differences between this transient metallic state and that seen across the thermally-driven insulator-metal transition. Suppressed low-frequency conductivity, Fano phonon lineshapes, and a mid-infrared absorption band point to polaronic transport. This is explained by noting that the photo-induced metallic state of 1T-TaS2 is one in which the Mott gap is melted but the lattice retains its low-temperature symmetry, a regime only accessible by photo-doping.

cond-mat.str-el↗