The quest for materials that become superconducting close to ambient conditions is a key topic of contemporary condensed matter research. We use ultrashort mid-infrared pulses to excite phonons and vibrational modes in unconventional superconductors and unleash superconductivity at temperatures higher than the equilibrium TC. So far, this phenomenon, known as light-induced superconductivity, has been observed in high-TC cuprates and organic superconductors. Recently, it was discovered that after mid-infrared excitation, a zero-resistance state appears in the alkali doped fulleride K3C60 and persists for several nanoseconds, holding a promise for applications in fast electronic devices. On-chip THz transport measurements, transient THz spectroscopy under extreme condition, and non-linear spectroscopies are routinely used to investigate the mechanisms behind these non-equilibrium superconducting states and their nature.
Reviews
Photo-induced superconductivity
Andrea Cavalleri
Contemporary Physics, 59, 31-46 (2018)
Abstract
Recent advances in laser technology have made it possible to generate of precisely shaped strong-field pulses at terahertz frequencies. These pulses are especially useful to selectively drive collective modes of solids, for example, to drive materials in a fashion similar to what done in the synthetic environment of optical lattices. One of the most interesting applications involves the creation of non-equilibrium phases with new emergent properties. Here, I discuss coherent control of the lattice to favour superconductivity at ‘ultra-high’ temperatures, sometimes far above the thermodynamic critical temperature Tc.
Key publications
Resonant enhancement of photo-induced superconductivity in K3C60
E. Rowe, B. Yuan, M. Buzzi, G. Jotzu, Y. Zhu, M. Fechner, M. Först, B. Liu, D. Pontiroli, M. Riccò, A. Cavalleri
Nature Physics, 19, 1821–1826 (2023)
Abstract
Photo-excitation at terahertz and mid-infrared frequencies has emerged as an effective way to manipulate functionalities in quantum materials, in some cases creating non-equilibrium phases that have no equilibrium analogue. In K3C60, a metastable zero-resistance phase was observed that has optical properties, nonlinear electrical transport and pressure dependencies compatible with non-equilibrium high-temperature superconductivity. Here we demonstrate a two-orders-of-magnitude increase in photo-susceptibility near 10 THz excitation frequency. At these drive frequencies, a metastable superconducting-like phase is observed up to room temperature. The discovery of a dominant frequency scale sheds light on the microscopic mechanism underlying photo-induced superconductivity. It also indicates a path towards steady-state operation, limited at present by the availability of a suitable high-repetition-rate optical source at these frequencies.
Superconducting nonlinear transport in optically driven high temperature K3C60
E. Wang, J. Adelinia, M. Chavez-Cervantes, T. Matsuyama, M. Fechner, M. Buzzi, G. Meier, A. Cavalleri
Nature Communications 14, 7233 (2023)
Abstract
Optically driven quantum materials exhibit a variety of non-equilibrium functional phenomena, which to date have been primarily studied with ultrafast optical, X-Ray and photo-emission spectroscopy. However, little has been done to characterize their transient electrical responses, which are directly associated with the functionality of these materials. Especially interesting are linear and nonlinear current-voltage characteristics at frequencies below 1 THz, which are not easily measured at picosecond temporal resolution. Here, we report on ultrafast transport measurements in photo-excited K3C60. Thin films of this compound were connected to photo-conductive switches with co-planar waveguides. We observe characteristic nonlinear current-voltage responses, which in these films point to photo-induced granular superconductivity. Although these dynamics are not necessarily identical to those reported for the powder samples studied so far, they provide valuable new information on the nature of the light-induced superconducting-like state above equilibrium Tc. Furthermore, integration of non-equilibrium superconductivity into optoelectronic platforms may lead to integration in high-speed devices based on this effect.
Amplification of Superconducting Fluctuations in Driven YBa2Cu3O6 + x
A. von Hoegen, M. Fechner, M. Först, N. Taherian, E. Rowe, A. Ribak, J. Porras, B. Keimer, M. Michael, E. Demler, and A. Cavalleri
Physical Review X, 12, 031008 (2022)
Abstract
In cuprate high-Tc superconductors, resonant excitation of certain lattice vibrations has been shown to induce transient terahertz reflectivity features suggestive of nonequilibrium superconductivity above the critical temperature Tc. A microscopic mechanism for these observations is still lacking. Here, time-resolved measurements of scattering-angle- and polarization-dependent second-harmonic generation in driven YBa2Cu3O6+x reveal a three-order-of-magnitude amplification of a 2.5-THz electronic mode, which is unique because of its symmetry, momentum, and temperature dependence. A theory for amplification of finite-momentum Josephson plasma polaritons, which are assumed to be well formed below Tc but incoherent throughout the pseudogap phase, explains all these observations. A theoretical solution for the Fresnel-Floquet reflection that starts from the coherently oscillating Josephson plasma polaritons provides a possible mechanism for the nonequilibrium superconductorlike terahertz reflectivity reported earlier. Beyond the immediate case of cuprates, this work underscores the role of nonlinear mode mixing to amplify fluctuating modes above the transition temperature in a wide range of materials.
Evidence for metastable photo-induced superconductivity in K3C60
M. Budden, T. Gebert, M. Buzzi, G. Jotzu, E. Wang, T. Matsuyama, G. Meier, Y. Laplace, D. Pontiroli, M. Riccò, F. Schlawin, D. Jaksch, A. Cavalleri
Nature Physics, 17, 611–618 (2021)
Abstract
Excitation of high-Tc cuprates and certain organic superconductors with intense far-infrared optical pulses has been shown to create non-equilibrium states with optical properties that are consistent with transient high-temperature superconductivity. These non-equilibrium phases have been generated using femtosecond drives, and have been observed to disappear immediately after excitation, which is evidence of states that lack intrinsic rigidity. Here we make use of a new optical device to drive metallic K3C60 with mid-infrared pulses of tunable duration, ranging between one picosecond and one nanosecond. The same superconducting-like optical properties observed over short time windows for femtosecond excitation are shown here to become metastable under sustained optical driving, with lifetimes in excess of ten nanoseconds. Direct electrical probing, which becomes possible at these timescales, yields a vanishingly small resistance with the same relaxation time as that estimated by terahertz conductivity. We provide a theoretical description of the dynamics after excitation, and justify the observed slow relaxation by considering randomization of the order-parameter phase as the rate-limiting process that determines the decay of the light-induced superconductor.
Photomolecular High-Temperature Superconductivity
M. Buzzi, D. Nicoletti, M. Fechner, N. Tancogne-Dejean, M. A. Sentef, A. Georges, T. Biesner, E. Uykur, M. Dressel, A. Henderson, T. Siegrist, J. A. Schlueter, K. Miyagawa, K. Kanoda, M.-S. Nam, A. Ardavan, J. Coulthard, J. Tindall, F. Schlawin, D. Jaksch, and A. Cavalleri
Physical Review X 10, 031028 (2020)
Abstract
The properties of organic conductors are often tuned by the application of chemical or external pressure, which change orbital overlaps and electronic bandwidths while leaving the molecular building blocks virtually unperturbed. Here, we show that, unlike any other method, light can be used to manipulate the local electronic properties at the molecular sites, giving rise to new emergent properties. Targeted molecular excitations in the charge-transfer salt κ-(BEDTTTF)2Cu[N(CN)2]Br induce a colossal increase in carrier mobility and the opening of a superconducting optical gap. Both features track the density of quasiparticles of the equilibrium metal and can be observed up to a characteristic coherence temperature T ≃ 50 K, far higher than the equilibrium transition temperature TC = 12.5 K. Notably, the large optical gap achieved by photoexcitation is not observed in the equilibrium superconductor, pointing to a light-induced state that is different from that obtained by cooling. First-principles calculations and model Hamiltonian dynamics predict a transient state with long-range pairing correlations, providing a possible physical scenario for photomolecular superconductivity.
Pressure tuning of light-induced superconductivity in K3C60
A. Cantaluppi, M. Buzzi, G. Jotzu, D. Nicoletti, M. Mitrano, D. Pontiroli, M. Riccò, A. Perucchi, P. Di Pietro, A. Cavalleri
Nature Physics, 14, 837–841 (2018)
Abstract
Optical excitation at terahertz frequencies has emerged as an effective means to dynamically manipulate complex materials. In the molecular solid K3C60, short mid-infrared pulses transform the high-temperature metal into a non-equilibrium state with the optical properties of a superconductor. Here we tune this effect with hydrostatic pressure and find that the superconducting-like features gradually disappear at around 0.3 GPa. Reduction with pressure underscores the similarity with the equilibrium superconducting phase of K3C60, in which a larger electronic bandwidth induced by pressure is also detrimental for pairing. Crucially, our observation excludes alternative interpretations based on a high-mobility metallic phase. The pressure dependence also suggests that transient, incipient superconductivity occurs far above the 150 K hypothesized previously, and rather extends all the way to room temperature.
Possible light-induced superconductivity in K3C60 at high temperature
M. Mitrano, A. Cantaluppi, D. Nicoletti, S. Kaiser, A. Perucchi, S. Lupi, P. Di Pietro, D. Pontiroli, M. Riccò, S. R. Clark, D. Jaksch, and A. Cavalleri
Nature, 530, 461–464 (2016)
Abstract
The non-equilibrium control of emergent phenomena in solids is an important research frontier, encompassing effects such as the optical enhancement of superconductivity. Nonlinear excitation
of certain phonons in bilayer copper oxides was recently shown to induce superconducting-like optical properties at temperatures far greater than the superconducting transition temperature, Tc. This effect was accompanied by the disruption of competing charge-density-wave correlations which explained some but not all of the experimental results. Here we report a similar phenomenon in a very different compound, K3C60. By exciting metallic K3C60 with mid-infrared optical pulses, we induce a large increase in carrier mobility, accompanied by the opening of a gap in the optical conductivity. These same signatures are observed at equilibrium when cooling metallic K3C60 below Tc (20 kelvin). Although optical techniques alone cannot unequivocally identify non-equilibrium high-temperature superconductivity, we propose this as a possible explanation of our results.
Optically-induced superconductivity in striped La2-xBaxCuO4 by polarization-selective excitation in the near infrared
D. Nicoletti , E. Casandruc, Y. Laplace, V. Khanna, C. R. Hunt, S. Kaiser, S. S. Dhesi, G. D. Gu, J. P. Hill, A. Cavalleri
Physical Review B, 90, 100503(R), (2014)
Abstract
We show that superconducting interlayer coupling, which coexists with and is depressed by stripe order in La1.885Ba0.115CuO4, can be enhanced by excitation with near-infrared laser pulses. For temperatures lower than Tc =13K,we observe a blue shift of the equilibriumJosephson plasma resonance, detected by terahertz-frequency reflectivity measurements. Key to this measurement is the ability to probe the optical properties at frequencies as low as 150 GHz, detecting the weak interlayer coupling strengths. For T > Tc a similar plasma resonance, absent at equilibrium, is induced up to the spin-ordering temperature TSO ≃ 40 K. These effects are reminiscent but qualitatively different from the light-induced superconductivity observed by resonant phonon excitation in La1.675Eu0.2Sr0.125CuO6.5. Importantly, enhancement of the below-Tc interlayer coupling and its appearance above Tc are preferentially achievedwhen the near-infrared pump light is polarized perpendicular to the superconducting planes, likely due to more effective melting of stripe order and the less effective excitation of quasiparticles from the Cooper pair condensate when compared to in-plane excitation.
Optically enhanced coherent transport in YBa2Cu3O6.5 by ultrafast redistribution of interlayer coupling
W. Hu, S. Kaiser, D. Nicoletti, C. R. Hunt, I. Gierz, M. C. Hoffmann, M. Le Tacon, T. Loew, B. Keimer & A. Cavalleri
Nature Materials, 13, 705–711 (2014)
Abstract
Nonlinear optical excitation of infrared active lattice vibrations has been shown to melt magnetic or orbital orders and to transform insulators into metals. In cuprates, this technique has been used to remove charge stripes and promote superconductivity, acting in a way opposite to static magnetic fields. Here, we show that excitation of large-amplitude apical oxygen distortions in the cuprate superconductor YBa2Cu3O6.5 promotes highly unconventional electronic properties. Below the superconducting transition temperature (Tc=50 K) inter-bilayer coherence is transiently enhanced at the expense of intrabilayer coupling. Strikingly, even above Tc a qualitatively similar eect is observed up to room temperature, with transient inter-bilayer coherence emerging from the incoherent ground state and similar transfer of spectral weight from high to low frequency. These observations are compatible with previous reports of an inhomogeneous normal state that retains important properties of a superconductor, in which light may be melting competing orders or dynamically synchronizing the interlayer phase. The transient redistribution of coherence discussed here could lead to new strategies to enhance superconductivity in steady state.
Optically induced coherent transport far above Tc in underdoped YBa2Cu3O6+δ
S. Kaiser, C. R. Hunt, D. Nicoletti, W. Hu, I. Gierz, H. Y. Liu, M. Le Tacon, T. Loew, D. Haug, B. Keimer, and A. Cavalleri
Physical Review B, 89, 184516 (2014)
Abstract
We report on a photoinduced transient state of YBa2Cu2O6+δ in which transport perpendicular to the Cu-O planes becomes highly coherent. This effect is achieved by excitation with mid-infrared optical pulses, tuned to the resonant frequency of apical oxygen vibrations, which modulate both lattice and electronic properties. Below the superconducting transition temperature Tc, the equilibrium signatures of superconducting interlayer coupling are enhanced. Most strikingly, the optical excitation induces a new reflectivity edge at higher frequency than the equilibrium Josephson plasma resonance, with a concomitant enhancement of the low-frequency imaginary conductivity σ2(ω). Above Tc, the incoherent equilibrium conductivity becomes highly coherent, with the appearance of a reflectivity edge and a positive σ2(ω) that increases with decreasing frequency. These features are observed up to room temperature in YBa2Cu2O6.45 and YBa2Cu2O6.5. The data above Tc can be fitted by hypothesizing that the light establishes a transient superconducting state over only a fraction of the solid, with a lifetime of a few picoseconds. Non-superconducting transport could also explain these observations, although one would have to assume transient carrier mobilities near 104 cm2/V sec at 100 K, with a density of charge carriers similar to the below-Tc superfluid density. Our results are indicative of highly unconventional nonequilibrium physics and open new prospects for optical control of complex solids.
Light induced Superconductivity in a Stripe-ordered Cuprate
D. Fausti, R.I. Tobey, N. Dean, S. Kaiser, A. Dienst, M.C. Hoffmann, S. Pyon, T. Takayama, H. Takagi and A. Cavalleri
Science, 331, 189-191 (2011)
Abstract
One of the most intriguing features of some high-temperature cuprate superconductors is the interplay between one-dimensional “striped” spin order and charge order, and superconductivity. We used mid-infrared femtosecond pulses to transform one such stripe-ordered compound, nonsuperconducting La1.675Eu0.2Sr0.125CuO4, into a transient three-dimensional superconductor. The emergence of coherent interlayer transport was evidenced by the prompt appearance of a Josephson plasma resonance in the c-axis optical properties. An upper limit for the time scale needed to form the superconducting phase is estimated to be 1 to 2 picoseconds, which is significantly faster than expected. This places stringent new constraints on our understanding of stripe order and its relation to superconductivity.
More publications
Two-fluid dynamics in driven YBa2Cu3O6.48
A. Ribak, M. Buzzi, D. Nicoletti, R. Singla, Y. Liu, S. Nakata, B. Keimer, A. Cavalleri
Physical Review B. 107, 104508 (2023)
Periodic dynamics in superconductors induced by an impulsive optical quench
P. E. Dolgirev, A. Zong, M. H. Michael, J. B. Curtis, D. Podolsky, A. Cavalleri and E. Demler
Nature Communications Physics 5, 234 (2022)
Higgs-mediated optical amplification in a non-equilibrium superconductor
M. Buzzi, G. Jotzu, A. Cavalleri, J. I. Cirac, E. A. Demler, B. I. Halperin, M. D. Lukin, T. Shi, Y. Wang, and D. Podolsky
Physical Review X 11, 011055 (2021)
A phase diagram for light-induced superconductivity in κ-(ET)2-X
M. Buzzi, D. Nicoletti, S. Fava, G. Jotzu, K. Miyagawa, K. Kanoda, A. Henderson, T. Siegrist, J. A. Schlueter, M.-S. Nam, A. Ardavan, A. Cavalleri
Physical Review Letters 127, 197002 (2021)
Pump Frequency Resonances for Light-Induced Incipient Superconductivity in YBa2Cu3O6.5
B. Liu, M. Först, M. Fechner, D. Nicoletti, J. Porras, B. Keimer, A. Cavalleri
Physical Review X 10, 011053 (2020)
Dynamical Superconductivity in a Frustrated Many-Body System
J. Tindall, F. Schlawin, M. Buzzi, D. Nicoletti, J. R. Coulthard, H. Gao, A. Cavalleri, M. A. Sentef, D. Jaksch
Physical Review Letters 125, 13 (2020)
Parametric resonance of Josephson plasma waves: A theory for optically amplified interlayer superconductivity in YBa2Cu3O6+x
M. H. Michael, A. von Hoegen, M. Fechner, M. Först, A. Cavalleri, and E. Demler
Physical Review B 102, 174505 (2020)
Magnetic-Field Tuning of Light-Induced Superconductivity in Striped La2−xBaxCuO4
D. Nicoletti, D. Fu, O. Mehio, S. Moore, A. S. Disa, G. D. Gu, and A. Cavalleri
Physical Review Letters,121, 267003 (2018)
Transiently enhanced interlayer tunneling in optically driven high-Tc superconductors
J. Okamoto, W. Hu, A. Cavalleri, L. Mathey
Physical Review B, 96, 144505 (2017)
Terahertz field control of interlayer transport modes in cuprate superconductors
F. Schlawin, A. S. D. Dietrich, M. Kiffner, A. Cavalleri, D. Jaksch
Physical Review B, 96 , 064526 (2017)
Optical melting of the transverse Josephson plasmon: a comparison between bilayer and trilayer cuprates
W. Hu, D. Nicoletti, A. V. Boris, B. Keimer and A. Cavalleri
Physical Reviev B, 95, 104508 (2017)
Theory of enhanced interlayer tunneling in optically driven high Tc superconductors
J.-i. Okamoto, A. Cavalleri, L. Mathey
Physical Review Letters, 117, 227001 (2016)
Dynamical decoherence of the light induced inter layer coupling in YBa2Cu3O6+δ
C. R. Hunt, D. Nicoletti, S. Kaiser, D. Pröpper, T. Loew, J. Porras, B. Keimer, A. Cavalleri
Physical Review B, 94, 224303 (2016)
Restoring interlayer Josephson coupling in La1.885Ba0.115CuO4 by charge transfer melting of stripe order
V. Khanna, R. Mankowsky, M. Petrich, H. Bromberger, S. A. Cavill, E. Möhr-Vorobeva, D. Nicoletti, Y. Laplace, G. D. Gu, J. P. Hill, M. Först, A. Cavalleri and S. S. Dhesi
Physical Review B 93, 224522 (2016)
Coherent modulation of the YBa2Cu3O6+x atomic structure by displacive stimulated ionic Raman scattering
R. Mankowsky, M. Först, T. Loew, J. Porras, B. Keimer, and A. Cavalleri
Physical Review B 91, 094308 (2015)
Wavelength-dependent optical enhancement of superconducting interlayer coupling in La1.885Ba0.115CuO4
E. Casandruc, D. Nicoletti, S. Rajasekaran, Y. Laplace, V. Khanna, G. D. Gu, J. P. Hill, and A. Cavalleri
Physical Review B, 91, 17 (2015)
Dynamical redistribution of phase fluctuations in bi-layer superconductors by periodic driving with an optical field
R. Höppner, B. Zhu, T. Rexin, A. Cavalleri, L. Mathey
Physical Review B 91, 104507 (2015)
Two distinct kinetic regimes for the relaxation of light-induced superconductivity in La1.675Eu0.2Sr0.125CuO4
C. R. Hunt, D. Nicoletti, S. Kaiser, T. Takayama, H. Takagi, and A. Cavalleri
Physical Review B 91, 020505(R) (2015)
Nonlinear lattice dynamics as a basis for enhanced superconductivity in YBa2Cu3O6.5
R. Mankowsky, A. Subedi, M. Först, S.O. Mariager, M. Chollet, H. Lemke, J. Robinson, J. Glownia, M. Minitti, A. Frano, M. Fechner, N. A. Spaldin, T. Loew, B. Keimer, A. Georges, A. Cavalleri
Nature 516, 71–73 (2014)
Melting of Charge Stripes in Vibrationally Driven La1.875Ba0.125CuO4: Assessing the Respective Roles of Electronic and Lattice Order in Frustrated Superconductors
M. Först, R. I. Tobey, H. Bromberger, S. B. Wilkins, V. Khanna, A. D. Caviglia, Y.-D. Chuang, W. S. Lee, W. F. Schlotter, J. J. Turner, M. P. Minitti, O. Krupin, Z. J. Xu, J. S. Wen, G. D. Gu, S. S. Dhesi, A. Cavalleri, and J. P. Hill
Physical Review Letters, 112, 157002 (2014)
Femtosecond x rays link melting of charge-density wave correlations and light-enhanced coherent transport in YBa2Cu3O6.6
M. Först, A. Frano, S. Kaiser, R. Mankowsky, C. R. Hunt, J. J. Turner, G. L. Dakovski, M. P. Minitti, J. Robinson, T. Loew, M. Le Tacon, B. Keimer, J. P. Hill, A. Cavalleri, and S. S. Dhesi
Physical Review B, 90, 184514 (2014)