Non-equilibrium superconductivity in driven alkali-doped fullerides

Giacomo Mazza1, 2, and Antoine Georges2, 1, 3

1
Centre de Physique Theorique, Ecole Polytechnique,
CNRS, Universite Paris-Saclay, 91128 Palaiseau, France
2
Coll`ege de France, 11 place Marcelin Berthelot, 75005 Paris, France
3
Department of Quantum Matter Physics, University of Geneva,
24 Quai Ernest-Ansermet, 1211 Geneva 4, Switzerland
We investigate the formation of non-equilibrium superconducting states in driven alkali-doped
fullerides A3 C60 . Within a minimal three-orbital model for the superconductivity of these materials,
arXiv:1702.04675v1 [cond-mat.supr-con] 15 Feb 2017

it was recently demonstrated theoretically that an orbital-dependent imbalance of the interactions

leads to an enhancement of superconductivity at equilibrium [M. Kim et al. Phys. Rev. B 94, 155152
(2016)]. We investigate the dynamical response to a time periodic modulation of this interaction
imbalance, and show that it leads to the formation of a transient superconducting state which
survives much beyond the equilibrium critical temperature Tc . For a specific range of modulation
frequencies, we find that the driving reduces superconductivity when applied to a superconducting
state below Tc , while still inducing a superconducting state when the initial temperature is larger
than Tc . These findings reinforce the relevance of the interaction-imbalance mechanism as a possible
explanation of the recent experimental observation of light-induced superconductivity in alkali-doped
fullerenes.

The optical stimulation of solids by means of strong
light pulses has opened new routes for the investigation
of collective phenomena in quantum materials [1]. A fas-
cinating one consists in inducing superconductivity (SC)
beyond the limits where it can be stabilized at equilib-
rium, which are set e.g. by temperature, external pres-
sure or doping concentration. A series of experiments
in different compounds revealed light-induced modifica-
tions of the electronic properties suggestive of the forma-
tion of a transient superconducting state extending above
the equilibrium critical temperature Tc [26]. Recently,
the remarkable observation of a superconducting-like re-
sponse above Tc in the molecular compound K3 C60 [6] en-
larged this experimental panorama and raised new ques-
tions about the possible mechanisms leading to transient
SC above Tc .
From the theoretical point of view, various mechanisms
have been investigated, such as the non-linear excitations
of phononic modes [5, 7] and their coupling to the elec-
tronic density [8] or the effective slowing-down of the elec-
tronic motion [9, 10]. While all these mechanisms lead
to an increase of the superconducting coupling which is
expected to provide a source of transient SC in a broad
class of superconductors, K3 C60 appears as a peculiar
case. Indeed, the absence of any enhancement or even
the suppression of SC below Tc reported in Ref. [6], to-
gether with the appearance of a transient response above
Tc is not fully understood within an effective SC cou-
pling enhancement. Furthermore, SC in alkali-doped ful-
lerides is strongly affected by the non-trivial interplay
between pairing, electronic correlations and orbital de-
grees of freedom [1115], requiring the investigation of
the mechanisms for transient SC within a proper theo-
retical framework taking this interplay into account.
A first step in this direction has been recently taken
by Kim et al. [16]. Working in the framework of the
low-energy electronic description of fullerides based on
the Jahn-Teller induced inversion of the effective Hunds
coupling [12], which provides one of the most successful
description of the unconventional superconducting prop-
erties of these materials [13], these authors demonstrated
that a specific orbital-dependent perturbation of the on-
site repulsive interactions does enhance SC at equilib-
rium. Such a perturbation was motivated by the pos-
sible modulations of the electronic interactions that re-
sult from the excitation of a local phononic mode, as
already demonstrated for other correlated organic com-
pounds [17, 18]. Furthermore, a first principle calcula-
tion [16] for K3 C60 revealed that the favorable perturba-
tion is indeed induced, under the assumption that light
excites the T1u mode [6], as a result of the structural and
electronic changes associated with this excitation.
This proposal relies entirely on equilibrium considera-
tions however, and this raises the outstanding question of
the relevance of this mechanism to the non-equilibrium
response of the system and to the transient light-induced
SC. In this work we address this question. We investigate
the non-equilibrium dynamics induced by the time- and
orbital- dependent modulation of the electron-electron
repulsion. We show that this results in a transient super-
conducting state, which can be induced when the system
is initially well above its equilibrium critical temperature.
The properties of this transient state dramatically de-
pend on the frequency of the modulation. In particular,
we uncover a regime of frequency in which the modula-
tion leads to the reduction of SC below Tc and to the
creation of SC above Tc , capturing an important aspect
of the aforementioned experimental observations.
The minimal description of strongly correlated super-
conductivity in alkali-doped fullerenes is given by the fol-
lowing three-bands model [12] arising from the t1u LUMO
states of the C60 molecule half-filled with electrons do-
 2

nated by the alkali atoms T=0 K T=58 K

3 0.06 = 0.1875 eV
(k)cka cka + 0.02
XX X
H= Hloc (i). (1) = 0.15 eV
k a=1 i

The local Hamiltonian Hloc (i) is of the Kanamori
type [19] and takes into account intra- and inter- or-
bital electron electron repulsion, spin-flip and pair hop-
ping terms, with a negative (inverted) Hunds cou-
pling JH resulting from the competition between the
Hunds coupling and the Jahn-Teller intramolecular in-
teractions [12].
We assume that, because the local electronic config-
urations couple to the square of the excited phonon
with frequency [17, 18], it leads to an oscillation of
the electronic interactions at a frequency 2 around a
value renormalized with respect to the equilibrium one
U (t) = U + U (1 cos 2t). First principle calcula-
tions [16] showed that in case of the excitation of the
T1u mode such renormalization is orbitally asymmetric
leading to the same value of U on two orbitals (x, y) and
an higher value on the third one (z). We include this per-
turbation in the model Hamiltonian Eq. (1) considering
the following time- and orbital- dependent interaction
U parameter for two driving frequencies = 0.1875 eV (blue
Ux,y (t) = U r(t) (1 cos 2t) ; Uz (t) = U, (2)
2 lines) and = 0.15 eV (red lines) at zero temperature (a)
where r(t) is a smooth ramping function defined as r(t) =
1/2 3/4 cos t/ + 1/4 cos3 t/ for t < and r(t) = 1
for t , being the ramping time during which the
modulation of the U is switched on.
We implemented and use the time-dependent
Gutzwiller approximation (tdGA) [20, 21] extended
to the multiband superconducting case [2224]. The
method is based on the variational ansatz for the time
evolved state
Y
|(t)i ' Pi (t) |0 (t)i , (3)
i
where |0 (t)i is an uncorrelated wavefunction describing
the coherent quasiparticle dynamics and P(t) is a pro-
jector onto the local Hilbert spaces giving the weights of
the local atomic multiplets. The dynamics of both quan-
tities are determined
R via the time-dependent variational
principle h(t)|it H|(t)i = 0. At equilibrium the
variational ansatz Eq. (3) is equivalent to the rotation-
ally invariant slave bosons technique [25] which has been
already successfully used to describe equilibrium strongly
correlated SC in the present model [26].
The method is extended to the finite-temperature case
by the introduction of a time dependent variational den-
sity matrix [27, 28]
(t) = P(t) (t)P(t) (4)
where the projector
P P(t) has the same definition as in (3)
and (t) = n pn |n (t)i hn (t)| is the density matrix
Psc
0.03 0.01
(a) (b)
0.000.0 1.0 2.0 3.00.000.0 1.0 2.0 3.0
time [ps] time [ps]
0.06
0.04 Psc0.04
0.02
P sc
0.00
0.02 0.0 0.4 0.8
U [eV]
1.2
(c)
0.000 40 80
T [K]
Figure 1. Panels (a)-(b): Dynamics of the global order
and T = 58 K > Tc ' 42 K (b). Panel (c): Transient or-
der parameter as a function of temperature. Color code as
in panel (a). Shaded area highlights the regime for which
SC is suppressed below Tc and created above. For T < Tc
(diamonds) where an almost steady value is reached during
the dynamics we extract this value taking a time average.
For T > Tc (circles) we take the value of the switched order
parameter at t = 3 ps. Dashed lines are guides to the eye.
Inset: Zero-temperature order parameter as a function of U .
The star indicates the values of parameters considered in this
work.
corresponding to a complete set of uncorrelated states
|n (t)i and a distribution pn . The dynamical equa-
tions for (4) are obtained by applying the finite tem-
perature generalization of the Dirac-Frenkel variational
principle [29]. They are solved numerically, with an ini-
tial condition corresponding to the equilibrium thermal
state. In the following we will consider a semicircular
density of states with a bandwidth W = 0.5 eV and
take U = 0.5 eV and JH = 0.02 eV. In the inset of
Fig. 1(c) we show that at equilibrium this corresponds to
a superconductor on the weak correlation side of the su-
perconducting dome determined by the electron-electron
repulsion U in the model Eq. (1). This is consistent with
e.g. the pressure dependence of Tc observed experimen-
tally for K3 C60 [30]. We take the modulation frequency
as an adjustable parameter in a range reasonably in-
cluding the typical frequencies of T1u modes and we fix
U/U = 0.1. We choose a ramping time = 0.9 ps.
 3

The following results do not depend qualitatively on this (a)

choice.
In Fig. 1(a)-(b), we plot the dynamics of the or- Psc 0.04
bital
P averaged amplitude of the order parameter Psc =
P
/3, P
= |hc, c, i|, for two different driving fre- (x,y) orb
sc sc
= 0.0625 eV (z) orb
quencies and at two temperatures below and above the
equilibrium critical temperature Tc ' 42 K (T = 0 K in
0.00
panel (a) and T = 58 K in panel (b)). A tiny symmetry (b)
breaking field is introduced for T > Tc to allow SC to
develop. Psc 0.04
For the larger driving frequency ( = 0.1875 eV), we
observe the increase of the superconducting order param- = 0.125 eV
eter at zero temperature and the formation of a finite 0.00
order parameter for T > Tc . This establishes that the (c)
SC-enhancement mechanism based on the imbalance of
U [16] does apply out of equilibrium. In particular the Psc 0.04
formation of a finite order parameter above Tc signals
that the initial normal metal becomes an unstable state
due to the increase of the critical temperature induced
by the average perturbation.
0.000.0 = 0.1875 eV 1.0 2.0 3.0
In contrast, a very different behaviour is observed when time [ps]
the driving frequency is lowered to = 0.15 eV. Start-
ing from the superconducting state, the order param- Figure 2. Zero-temperature dynamics of the order parame-
eter undergoes a decrease instead of the expected in- ter amplitude for x, yorbitals (red lines) and zorbital (blue
crease. On the other hand, a finite order parameter is lines). Driving frequencies = 0.0625 eV (a), = 0.125 eV
still established above the critical temperature, though (b) and = 0.1875 eV (c). Dashed lines: unmodulated dy-
its amplitude is smaller than the one established for namics after the switching of a constant imbalance of U equal
to the average of the periodic modulation (see text). The
= 0.1875 eV.
arrows represent the expected equilibrium order parameters
In panel (c) we compare the transient order parameter corresponding to the average interaction imbalance.
as a function of the initial temperature to the equilibrium
one. The former is extracted as a timeRaverage over a time
tmax
interval t = tmax tmin , P sc = tmin d Psc ( )/t,
quency = 2 reflect the periodical modulation of U
for T = 0 K while we estimate it for T > Tc from the
and are absent in the case of the unmodulated dynamics
value it takes at t = 3 ps. For = 0.1875 eV, the non-
(dashed lines). A larger order parameter is established in
equilibrium perturbation enhances SC for all tempera-
the latter case. The two dynamics become equivalent at
tures, up to about T . 100 K, way above equilibrium
larger driving frequency ( = 0.1875 eV in panel (c)), the
Tc . On the contrary, the = 0.15 eV case shows a re-
only difference being the fast oscillations of small ampli-
markable suppression of SC for T < Tc and the formation
tude in the modulated case. The unexpected behaviour
of SC up to temperatures slightly below the previous case
mentioned above at intermediate frequencies is clearly
T . 90 K.
seen on panel (b) of Fig. 2 for the driving frequency
In order to obtain insights into these results, we study
= 0.125 eV where the periodic modulation leads in
the orbital resolved dynamics of the zero-temperature su-
this case to an almost complete suppression of the super-
perconductivity at three increasing frequencies (Fig. 2).
conducting order.
We compare it to the time evolution obtained by an
imbalance of U equal to the average of the modulated The non-monotonic response of the transient state to
case Eq. (2) switched on during the same ramp time the frequency of the interaction modulation is summa-
Ux,y (t) = U r(t)U/2, hereafter called unmodulated dy- rized in Fig. 3, where we report the existence of a fre-
namics. quency range 0.09 eV . . 0.16 eV in which SC is
The imbalance of U lifts the orbital degeneracy be- suppressed instead of enhanced. This frequency range is
tween the components of the superconducting order pa- comprised between a lower frequency region in which the
rameter Psc
. For the slowest driving frequency ( = enhancement of SC is smaller than the case of the unmod-
0.0625 eV in panel (a)) the order parameter components ulated dynamics and an higher frequency region in which
display an oscillating behaviour around an almost steady the perturbation becomes completely anti-adiabatic with
value. A global enhancement is observed, though smaller respect to the periodic change of U and thus coincides
than what is expected from the equilibrium imbalanced with the unmodulated one.
case (see arrows in Fig. 2). The fast oscillations of fre- We trace back the origin of the behaviour observed
 4

doublons. Such process becomes resonant in the inter-

1.5 mediate frequency regime (panel (c)) where the strong
(d) amplification of the doublons oscillations is observed. As
(b)
1.0
P sc /Psc, 0
shown by the dynamics of the systems internal energy
E(t) = hHi (panel (e)), such a large amount of excitations
0.5 leads to a sizable energy absorption which suppresses SC
with respect to what is expected for the unmodulated
(a) (c)
dynamics (dashed line in panel (a)).
0.00.1 0.2 0.3 0.4 0.5 We find that the origin of such behaviour is the res-
2 [eV] onance between the modulation frequency 2 and the
spectrum of the non-equilibrium excitations of the or-
0.4 = 0.0625
(x,y)
eV = 0.125 eV = 0.1875 eV
bitally imbalanced populations of doublons induced by
(z)
0.3 the asymmetric interaction (shaded area in panel (a)).
Such spectrum is defined from the frequency spectrum
D

0.2 FD of the dynamics of doublons following the sudden

switch of a fixed U imbalance, Ux,y (t) = U (t)U [31].
(b) (c) (d)
0.10.0 1.0 0.0 1.0 0.0 1.0
We compute FD at fixed U and then integrate over a
window equal to the amplitude of the interaction imbal-
time [ps] time [ps] time [ps] ance considered in the modulated dynamics 0 < U <
-2.50 (c)
0.05 eV. The resulting spectrum has a broad three peaks
structure which exactly matches the frequency region for
which SC is suppressed. An investigation of the structure
[eV]

-2.55 of the spectrum revealed that the two side-bands mainly

depend on the value of JH and disappear for JH = 0
E

(e) (b) (d) indicating processes of inter-orbital origin. On the other

-2.600.0 1.0 2.0
time [ps]
Figure 3. Panel (a): Stationary zero-temperature supercon-
ducting order parameter normalized by the equilibrium value
as a function of the driving frequency. Dashed lines: station-
ary order parameter for the constant U -imbalance dynamics.
Arrows show the transient states considered in Fig. 2 and in
panels (b)-(d). Dotted line represents the equilibrium value.
The shaded area represents the spectrum of excitations of the
non-equilibrium doublons (see text). Panels (b)-(d): Dynam-
ics of the number of average number of intra-orbital double
occupations for the driving frequencies = 0.0625 eV (b),
= 0.125 eV (c) and = 0.1875 eV (d) and the constant
U -imbalance (dashed lines). Panel (e): Dynamics of the in-
ternal energies for the three frequencies in panels (b)-(d) (see
arrows).
in the different regimes to the doublons excitations in-
duced by the periodic modulation of U . Panels (b)-(d)
of Fig. 3 display the dynamics of the double occupancies
on each orbital D = hn n i for the three frequen-
cies representative of the different regimes. Due to the
asymmetric value of the interaction the number of pairs
is enhanced in the (x, y) orbital and lowered on the (z)
one. However the dynamics is markedly different in the
different regimes of frequency. At small and large fre-
quencies (panel (b) and (d)), the dynamics closely follows
the unmodulated one with superimposed 2 oscillations
indicating the creation of double occupancies on top of
the orbitally imbalanced populations of non-equilibrium
3.0 hand, the central peak weakly depends on JH and de-
creases with U (not shown) suggesting processes within
the renormalized quasi-particle bandwidth as expected
by the fact that the number of excited doublons is in a
small quench regime (U/U = 0.1).
We finally observe that away from the resonance a
small energy absorption is present for the slow driving
case, whereas it is almost negligible for the fast one. This
reflects in the mismatch between the modulated and the
unmodulated dynamics for frequencies smaller than the
resonance.
The above results show that the frequency dependence
of the transient superconducting state presented in Fig. 1
as a function of the initial temperature is due to the com-
petition between the average interaction asymmetry and
the doublons excitations created by the U -modulation.
The former favours the formation of a transient super-
conducting state with a larger order parameter extending
much beyond the equilibrium critical temperature, while
the latter can induce the suppression of SC due to the
energetic cost in creating pairs in a correlated system.
Nonetheless, this does not preclude SC to appear above
equilibrium Tc and the signature of a transient SC state
above Tc may survive also in the region where pairs are
resonantly excited, as shown in Fig. 1 for = 0.15 eV.
This realizes an unexpected dynamical response for which
SC is dynamically extended beyond Tc and not enhanced
for T < Tc .
In conclusion we have investigated the non-equilibrium
dynamics of a minimal model describing SC in alkali-
doped fullerides subject to the orbital asymmetric peri-

odic modulation of the local interaction energies. This
perturbation may result from the light-induced excita-
tion of a local vibrational mode and is known to enhance
SC at equilibrium [16]. We showed that this leads to
the dynamical formation of a superconducting state ex-
tending beyond the equilibrium critical temperature Tc .
Due to the correlated nature of such systems we showed
that the transient state, while extending SC beyond Tc ,
may show no significant enhancement of the supercon-
ducting properties below Tc where a SC suppression can
even occour. This captures a non-trivial observation in
the light-induced response of K3 C60 which validates the
mechanism as a possible source of light-induced SC in
these systems.
Acknowledgments. We thank Minjae Kim, A. Caval-
leri, M. Fabrizio, M. Capone and H. Strand for insightful
discussions. This work was support by the European Re-
search Council (ERC-319286 QMAC).
giacomo.mazza@polytechnique.edu
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