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

Psc
The local Hamiltonian Hloc (i) is of the Kanamori
type [19] and takes into account intra- and inter- or-
0.03 0.01
bital electron electron repulsion, spin-flip and pair hop-
ping terms, with a negative (inverted) Hunds cou-
(a) (b)
pling JH resulting from the competition between the 0.000.0 1.0 2.0 3.00.000.0 1.0 2.0 3.0
Hunds coupling and the Jahn-Teller intramolecular in-
teractions [12]. time [ps] time [ps]
We assume that, because the local electronic config-
urations couple to the square of the excited phonon 0.06
with frequency [17, 18], it leads to an oscillation of 0.04 Psc0.04
the electronic interactions at a frequency 2 around a 0.02
value renormalized with respect to the equilibrium one P sc
0.00
U (t) = U + U (1 cos 2t). First principle calcula- 0.02 0.0 0.4 0.8
U [eV]
1.2
tions [16] showed that in case of the excitation of the
T1u mode such renormalization is orbitally asymmetric
(c)
leading to the same value of U on two orbitals (x, y) and 0.000 40 80
an higher value on the third one (z). We include this per-
turbation in the model Hamiltonian Eq. (1) considering T [K]
the following time- and orbital- dependent interaction
Figure 1. Panels (a)-(b): Dynamics of the global order
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) = and T = 58 K > Tc ' 42 K (b). Panel (c): Transient or-
der parameter as a function of temperature. Color code as
1/2 3/4 cos t/ + 1/4 cos3 t/ for t < and r(t) = 1 in panel (a). Shaded area highlights the regime for which
for t , being the ramping time during which the SC is suppressed below Tc and created above. For T < Tc
modulation of the U is switched on. (diamonds) where an almost steady value is reached during
We implemented and use the time-dependent the dynamics we extract this value taking a time average.
Gutzwiller approximation (tdGA) [20, 21] extended For T > Tc (circles) we take the value of the switched order
to the multiband superconducting case [2224]. The parameter at t = 3 ps. Dashed lines are guides to the eye.
method is based on the variational ansatz for the time Inset: Zero-temperature order parameter as a function of U .
The star indicates the values of parameters considered in this
evolved state work.
Y
|(t)i ' Pi (t) |0 (t)i , (3)
i
corresponding to a complete set of uncorrelated states
where |0 (t)i is an uncorrelated wavefunction describing |n (t)i and a distribution pn . The dynamical equa-
the coherent quasiparticle dynamics and P(t) is a pro- tions for (4) are obtained by applying the finite tem-
jector onto the local Hilbert spaces giving the weights of perature generalization of the Dirac-Frenkel variational
the local atomic multiplets. The dynamics of both quan- principle [29]. They are solved numerically, with an ini-
tities are determined
R via the time-dependent variational tial condition corresponding to the equilibrium thermal
principle h(t)|it H|(t)i = 0. At equilibrium the state. In the following we will consider a semicircular
variational ansatz Eq. (3) is equivalent to the rotation- density of states with a bandwidth W = 0.5 eV and
ally invariant slave bosons technique [25] which has been take U = 0.5 eV and JH = 0.02 eV. In the inset of
already successfully used to describe equilibrium strongly Fig. 1(c) we show that at equilibrium this corresponds to
correlated SC in the present model [26]. a superconductor on the weak correlation side of the su-
The method is extended to the finite-temperature case perconducting dome determined by the electron-electron
by the introduction of a time dependent variational den- repulsion U in the model Eq. (1). This is consistent with
sity matrix [27, 28] e.g. the pressure dependence of Tc observed experimen-
(t) = P(t) (t)P(t) (4) tally for K3 C60 [30]. We take the modulation frequency
as an adjustable parameter in a range reasonably in-
where the projector
P P(t) has the same definition as in (3) cluding the typical frequencies of T1u modes and we fix
and (t) = n pn |n (t)i hn (t)| is the density matrix 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 3.0 hand, the central peak weakly depends on JH and de-
time [ps] creases with U (not shown) suggesting processes within
the renormalized quasi-particle bandwidth as expected
Figure 3. Panel (a): Stationary zero-temperature supercon- by the fact that the number of excited doublons is in a
ducting order parameter normalized by the equilibrium value small quench regime (U/U = 0.1).
as a function of the driving frequency. Dashed lines: station- We finally observe that away from the resonance a
ary order parameter for the constant U -imbalance dynamics. small energy absorption is present for the slow driving
Arrows show the transient states considered in Fig. 2 and in case, whereas it is almost negligible for the fast one. This
panels (b)-(d). Dotted line represents the equilibrium value.
reflects in the mismatch between the modulated and the
The shaded area represents the spectrum of excitations of the
non-equilibrium doublons (see text). Panels (b)-(d): Dynam- unmodulated dynamics for frequencies smaller than the
ics of the number of average number of intra-orbital double resonance.
occupations for the driving frequencies = 0.0625 eV (b), The above results show that the frequency dependence
= 0.125 eV (c) and = 0.1875 eV (d) and the constant of the transient superconducting state presented in Fig. 1
U -imbalance (dashed lines). Panel (e): Dynamics of the in- as a function of the initial temperature is due to the com-
ternal energies for the three frequencies in panels (b)-(d) (see petition between the average interaction asymmetry and
arrows).
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
in the different regimes to the doublons excitations in- much beyond the equilibrium critical temperature, while
duced by the periodic modulation of U . Panels (b)-(d) the latter can induce the suppression of SC due to the
of Fig. 3 display the dynamics of the double occupancies energetic cost in creating pairs in a correlated system.
on each orbital D = hn n i for the three frequen- Nonetheless, this does not preclude SC to appear above
cies representative of the different regimes. Due to the equilibrium Tc and the signature of a transient SC state
asymmetric value of the interaction the number of pairs above Tc may survive also in the region where pairs are
is enhanced in the (x, y) orbital and lowered on the (z) resonantly excited, as shown in Fig. 1 for = 0.15 eV.
one. However the dynamics is markedly different in the This realizes an unexpected dynamical response for which
different regimes of frequency. At small and large fre- SC is dynamically extended beyond Tc and not enhanced
quencies (panel (b) and (d)), the dynamics closely follows for T < Tc .
the unmodulated one with superimposed 2 oscillations In conclusion we have investigated the non-equilibrium
indicating the creation of double occupancies on top of dynamics of a minimal model describing SC in alkali-
the orbitally imbalanced populations of non-equilibrium doped fullerides subject to the orbital asymmetric peri-
5

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