Articles

https://doi.org/10.1038/s41566-019-0470-y

Lightwave-driven gapless superconductivity

and forbidden quantum beats by terahertz
symmetry breaking
X. Yang   1, C. Vaswani   1, C. Sundahl2, M. Mootz3, L. Luo1, J. H. Kang2, I. E. Perakis3, C. B. Eom2
and J. Wang   1*

Light-induced supercurrents chart a path forward for the electromagnetic design of emergent materials phases and collec-
tive modes for quantum engineering applications. However, controlled spatial–temporal modulation of the complex order
parameter characterizing such non-equilibrium macroscopic quantum states remains elusive. Such ultrafast phase-amplitude
modulation can manifest via high harmonic modes beyond those allowed by equilibrium symmetries. Here, we drive moving con-
densate states via subcycle dynamical symmetry breaking achieved with nonlinear oscillating terahertz photocurrents. These
non-equilibrium macroscopic quantum states with broken inversion symmetry are controlled via Cooper pair acceleration by
asymmetric and multi-cycle terahertz photoexcitations. The observed supercurrent-carrying states evolve during a lightwave
cycle and exhibit three distinguishing features: Anderson pseudo-spin precessions forbidden by equilibrium symmetry, strong
high harmonic coherent oscillations assisted by pairing and long-lived gapless superfluidity with minimal condensate quench.
Lightwave tuning of persistent photocurrents can be extended for quantum control of unconventional superconductors and
topological matter, with implications on quantum gate and sensing functionalities.

U
ltrafast nonlinearity in quantum systems is emerging as a
frontier for enabling laser-driven many-body correlation phe-
nomena1–12. So far, strong coupling of superconductors (SCs)
to intense terahertz (THz) pulses has revealed collective modes3–6,8,13
and a gapless quasiparticle (QP) metastable phase hidden beneath the
SCs7, for example. One standard model for understanding ultrafast
SC condensate coupling to an a.c. electric field, illustrated in Fig. 1a,
is Anderson pseudo-spin precession, s k (t ) (indicated by arrows).
This precession is driven by even nonlinear couplings, O(A2n), of
the vector electromagnetic potential A(t), which are the only ones
allowed by equilibrium Bardeen–Cooper–Schrieffer (BCS) symme-
t
ps (R, t ) = −2e A(R, t ) + ∇R ζ (R, t ) = 2e ∫ E eff (R, t )dt (1)
−∞
where 2e is the Cooper pair charge and Eeff(R,t) (see Methods, equa-
tion (3)) is the effective pulse that drives the light-induced CM
motion. Furthermore, such local field gauge-invariant superfluid
momentum can remain finite long after the pulse because THz-driven
nonlinear photocurrent sources and spatial variations determine an
effective asymmetric oscillating electric field inside the SC during
∞
THz pulse propagation that satisfies the property ∫ dτ E eff (τ ) ≠ 0
−∞
(ref. ). Such an effective pulse will drive persistent condensate flow
17

try1,2,14,15. Here we explore a different nonlinear mechanism—peri-
odic and asymmetric acceleration of Cooper pair centre-of-mass
(CM) motion driven by phase-locked multi-cycle THz electric-field
pulses. We show that experimental manifestations of such lightwave
acceleration of a macroscopic quantum state include strong odd
(forbidden) Anderson pseudo-spin high harmonic (HH) generation
nonlinearities enabled by subcycle symmetry breaking and gapless
superfluidity. The latter results from transient changes in the pair-
ing for sufficiently strong THz gauge fields corresponding to finite
Cooper pair CM momentum. This coherent asymmetric THz field
driving of the condensate does not rely on resonant excitation of
QPs or bandstructure details2,16, but rather on transient breaking of
equilibrium inversion symmetry and nonlinear photocurrents. This
is achieved by introducing a preferred direction parallel to the oscil-
lating electric field, which leads to (k + ps(t)↑, −k + ps(t)↓) Cooper
pairs, with spatially–temporally modulated superfluid CM momen-
tum ps(R,t). The latter is created during the pulse (Fig. 1a, red line),
via periodic acceleration of the SC condensate by the oscillating THz
field and via spatial variations in the SC order parameter phase ζ:
if disorder is minimized in sufficiently clean SCs.
We note two smoking-gun signatures of the periodically driven,
supercurrent-carrying macroscopic state. First, as illustrated in
Fig. 1a, the coexistence and interference (white dashed arrows) in
a pump–probe two-pulse experiment of quantum transport, ps(t)
(red lines), with even-order nonlinearity, O(A2n) (green lines),
can result in new forbidden Anderson pseudo-spin modes due
to dynamical symmetry breaking, for example, coherent pseudo-
spin oscillation (PSO) at 3ωpump. However, only even-order PSO
nonlinearities have been considered so far, limited to the O(A2) at
2ωpump observed experimentally, corresponding to a perturbative
expansion4. Second, in a moving condensate, vs(t ), the SC order
parameter ΔSC(t) is no longer equal to the QP excitation energy,
QP
E min (t ) ≈ ΔSC (t )−pF ⋅ vs(t ), where pF is the Fermi vector. To illustrate
this, Fig. 1b compares the QP dispersion between the equilibrium
BCS state (left), with finite energy gap 2ΔSC, and the current-carry-
ing state (right) at critical Cooper pair velocity, vs(t ) ⋅ pF = Δ SC. The
QP
latter state is gapless at k points with vanishing E min ; that is, it costs
zero energy to excite QPs, although the order parameter ΔSC(t) and

1
Department of Physics and Astronomy, Iowa State University and Ames Laboratory – USDOE, Ames, IA, USA. 2Department of Materials Science and
Engineering, University of Wisconsin–Madison, Madison, WI, USA. 3Department of Physics, University of Alabama at Birmingham, Birmingham, AL, USA.
*e-mail: jgwang@iastate.edu

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Articles NATurE PHoToniCS

a THz electric field

c
Pseudospin
Multi-cycle pump
A2(ω)
0.2 ω0.5THz,E = 11.5 kV cm–1
Temperature (K)
5 10 15
Quantum 1.0

Osc. amp. (a.u.)

ΔE/E
interference Tc
0.1 0.5
–k
Supercurrent
k 0
A(ω) T = 4.1 K Experiment
0
0 5 10 15
∆tpp (ps)

b Equilibrium Supercurrent flowing

d tgate (ps) e
4 Net

J (10 A cm )
10 2nd

2
1 1st 2 current
Theory
3

6
0

Osc. amp. (a.u.)

Gauge-invariant
5 –2
5 4th –4
Asymmetric
0.1 Symmetric
3rd
0 10 20 LPS model

(Δ − Δ0)/Δ0 (%)
ε(P)/ΔSC

Periodic
0 2ΔSC 0 2
nonlinear 0.01
currents

–5 –5 f
2nd
100 4th 0 5 10 15
Theory 1

Δ(ω) (a.u.)
3rd
–10 0
10–2

(×10–5)
–2
–2 –2 –2 –4
0 –2 0 0 10–4 –6
0 2
2 P/P
P/P P/PF F P/PF 10–6 0
F
1 2 3 4 5 6 0 5 10 15
ω/ωpump ∆tpp (ps)

Fig. 1 | Pseudo-spin coherent oscillations forbidden by equilibrium symmetry and strong HH generation nonlinearities. a, Experimental schematics:
quantum dynamics of Anderson pseudo-spins (gradient arrows from red to blue) in a supercurrent-carrying macroscopic quantum state with time-
dependent CM momentum pairing induced by an intense multi-cycle THz driving electric field. b, QP energy dispersion ε(P) of the fully gapped
equilibrium state (left) and the gapless current-carrying state with critical condensate flow vs ≈ 3.15 × 104 cm s−1 along the x axis (right) in our Nb3Sn
sample. Note that ΔSC/EF = 0.4 (instead of 0.002) in Nb3Sn is used to better visualize the partial gap closing (see Supplementary Information). Here EF is
the Fermi energy. c, Pump-induced change ΔE/E for a narrowband driving E field centred at 0.5 THz (2.1 meV) shows pronounced quantum beats. Inset:
oscillation amplitudes vanish at the critical temperature, Tc. d, Quantum beat pump–probe experimental spectra showing PSO modes at 2ωpump, 3ωpump
and 4ωpump and THz-driven supercurrent at ωpump; the amplitudes are plotted in a log scale to highlight the higher-order PSO harmonics. Inset: simulated
net supercurrent, marked by an arrow, produced by a multi-cycle THz pulse as in the experiment in c,d, driving a circuit model (see Supplementary
Information). e,f, Simulated order parameter dynamics in time (e) and frequency (f) domains, obtained by using the gauge-invariant quantum kinetic
theory summarized in the Supplementary Information, with asymmetric (red) and symmetric (green) effective input THz pulses, and the linearized
pseudo-spin (LPS) model (black). The amplitude of the forbidden 3ωpump peak is enhanced by increasing asymmetric THz driving, while even PSO
harmonics are less sensitive to this.

superfluid density ns(t) remain finite. A supercurrent-carrying gap-
less state is difficult to realize in equilibrium, due in part to heating
of electric contacts in the presence of the large current and impurity
scattering. Although an equilibrium gapless state has been inferred
in tunnelling spectroscopy of d.c.-biased SC nanowires18 and also
induced as a Fulde–Ferrell–Larkin–Ovchinnikov state, coherent
tuning of gapless superfluidity19 is difficult using these equilibrium
methods. Here it is achieved by nonlinear lightwave acceleration of
time-dependent supercurrents (Fig. 1a).
In this Article, we drive a non-thermal transition from the equi-
librium BCS state to a long-lived, supercurrent-carrying macro-
scopic quantum state in sufficiently clean Nb3Sn. This is achieved
by non-contact alternating current-bias using the sub-gap THz
carrier wave of the light electric field7,20. The subcycle dynamical
symmetry breaking manifests itself via the emergence of forbid-
den third-order PSOs, interaction-enhanced strong fourth-order
HH generation nonlinearities and light-induced gapless super-
conductivity. Our results are consistent with the predictions of
a quantum kinetic nonlinear calculation using a gauge-invariant
density matrix.
Forbidden Anderson pseudo-spin and HH oscillations
The pseudo-spin coherent precession measured in a Nb3Sn film21
(see Methods) are shown in Fig. 1c. The SC state is driven by an
ETHz = 11.5 kV cm−1 sub-gap THz field with central frequency
ωpump =  0.5 
THz (2.1  meV), well below the pair-breaking gap
2ΔSC = 1.2 THz at 4.1 K. The dynamical symmetry breaking super-
current and nonlinear effects become observable in a THz pump and
THz probe experiment, by measuring the differential THz transmis-
sion ΔE/E0 as a function of pump–probe time delay. Such two-pulse
experiment improves the sensitivity and resolution by subtract-
ing the linear background in emission that masks the nonlinear
quantum dynamics. The coherent dynamics reveals a pronounced
quantum beating superimposed on a slow amplitude change, which
vanishes above the critical temperature Tc ≈ 16 K (inset, Fig. 1c). The
origin of the oscillatory behaviour of ΔE/E0 is demonstrated by its
Fourier transformation, shown in Fig. 1d. Besides the conventional
2ωpump mode (the same as third harmonic generation, THG, in emis-
sion1,4; see Supplementary Information), the pump–probe nonlinear
spectrum directly observed here displays three new strong peaks:
(1) an inversion symmetry-forbidden, third-harmonic PSO mode
at 3ωpump, (2) a strong fourth-harmonic PSO mode at 4ωpump and
(3) a narrow first-order peak at the fundamental driving frequency,
indicative of the build-up of a long-lived supercurrent (inset,
Fig. 1d). Odd-order PSO peaks are the hallmark of symmetry
breaking, here induced by THz field–SC condensate coupling.
Furthermore, the fourth to second order peak ratio is ~10%, 1,000
times bigger than in the standard model1, 1/12(πeE)/(2pFω)2 ≈ 10−4.

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NATurE PHoToniCS Articles
a c d 1.0
60 2 2nd

Amp. (a.u.)
Integral (a.u.)
Single-cycle Probe 1st Theory
Multi-cycle ω1THz 20 1st
0 2nd

Amp. (a.u.)
40 Multi-cycle ω0.5THz 3rd 4th
–2
0.5
ETHz (kV cm–1)

20
0.5 1.0 1.5 2.0
–2 0 2 4 ω (THz)
0 tgate (ps) 3rd 4th
Multi-cycle ω0.5THz

Integration of normalized ETHz (t ) (a.u.)

–20 0
47 kV cm–1 e 1.0

Amp. (a.u.)
–40 –1 10 1st 2nd
60 kV cm Multi-cycle, 1st
11.5 kV cm–1 ω0.5THz Dirty NbN
–60

Amp. (a.u.)
0.5 1 2 3 4
0 5 10 15 20 2nd
tgate (ps) Nonlinear coupling Multi-cycle ω1THz
b 1.5 Multi-cycle, ω1THz 0
2∆SC 0
f
σ1 (104 Ω–1 cm–1)

1.0 Single-cycle ω1THz

1.0

Amp. (a.u.)
Single-cycle pulse 1st 2nd
0.5 0.5

–10
0 0
2 4 6 8 10 0 10 20 30 40 1 2 3 4
ω (meV) tgate (ps) ω (THz)

Fig. 2 | Lightwave-driven collective modes with different THz nonlinear and asymmetric driving. a, Three different THz temporal waveforms Epump(t)
measured inside a nonlinear crystal: single-cycle pulse centred at 1 THz (grey) and multi-cycle pulses centred at 0.5 THz (red) and 1 THz (blue). b, Plots of
t
their spectra Epump(t) and comparison to the static σ1(ω) (open circles) at 4.1 K. c, Effective THz pump field nonlinear coupling by integration ∫−∞ dτ E eff(τ )
using the normalized THz pump pulses measured inside a nonlinear crystal shows different tilting and oscillation cycles. Inset: integral of the THz probe
pulse. d–f, Quantum beating spectra of experimentally measured coherent THz pump–probe dynamics of the supercurrent-carrying quantum state under
the three different THz driving fields shown in a: multi-cycle ω0.5THz (d), multi-cycle ω1THz (e) and single-cycle (f). Even- and odd-order collective modes are
marked by dashed lines. Inset in d shows the pump–probe spectrum obtained from the simulated coherent ΔE/E dynamics using the multi-cycle 0.5 THz
pump waveform in a (red line) exhibits collective modes fully consistent with the experiment (Supplementary Fig. 6). Inset in e shows PSO spectrum of a
dirty limit NbN SC sample at 4.1 K driven by the multi-cycle 1 THz pulse in a (blue line) exhibits negligible supercurrent peak at the driving frequency.

Figure 1e (time domain) and Fig. 1f (frequency domain) com- nonlinear asymmetric coupling, we compute the effective nonlin-
t
pare the experimental results to those for our gauge-invariant ear pulse integral ∫ dτ E eff (τ ) by inputting the THz pump pulse
−∞
quantum kinetic theory with ps(t) ≠ 0. By using an effective, slightly waveforms detected via electrooptic sampling in a <110> ZnTe
asymmetric sub-gap THz driving of the SC (red lines), we obtain crystal. Figure 2c clearly shows that the intense THz pulses used
both the forbidden mode at 3ωpump and strong even harmonics, here as pump exhibit a non-zero integral of Eeff(τ) when propagat-
with a gigantic, interaction-enhanced, fourth to second order ratio ing in a nonlinear crystal, seen as a tilting of the temporal profile.
of ~10%, comparable to that in the experiment. These HH peaks are In contrast, the weak probe THz pulse exhibits zero integral over
vanishingly small in the linearized pseudospin (LPS) model (black time with negligible tilting (inset, Fig. 2c). Note that, in the SC, a
lines). Note that the exact mechanism and details for generating quantitative analysis of the gauge-invariant coupling of THz fields
ps(t) do not affect the above identifications. We also compare our and superfluid momentum ps(t) needs to also include longitudinal
results to the theoretical results for symmetric THz driving (green responses from spatial variations of the order parameter phase and
lines), where ps ≈ 0 after the THz pump, which suppresses the 3ωpump chemical potential, as seen in equations (3) and (4) (see Methods).
mode (Fig. 1f) since ps(t) oscillates symmetrically between positive We point out four key observations when comparing the pump–
and negative values. These theoretical results indicate that the odd probe responses for the three different pump pulses in Fig. 2a,b.
coherent PSOs are controlled by the THz effective field pulse shape First, the 0.5 THz excitation clearly reveals first to fourth PSO
and SC phase spatial fluctuations (equation (1)), while the even har- modes (Fig. 2d), while the 1 THz excitation does not show third-
monic peak strength mostly depends on the pairing interaction and and fourth-order HH peaks (Fig. 2e). Comparing the 0.5 THz (red)
lightwave acceleration beyond the LPS model. These results under- and 1 THz (blue) pump pulses (Fig. 2a), the former has a compa-
pin the interplay between subcycle dynamical symmetry breaking rable coupling to Anderson pseudo-spin precessions, that is deter-
due to ps(t) and interaction-enhanced HH generation nonlinearities mined by A(t)2 ∝ E2/ω2, but higher asymmetry, seen as larger tilting
in determining the light-driven SC ultrafast nonlinear dynamics. of the time integral that is indicative of the nonlinear coupling of
The asymmetric and multi-cycle THz driving used here is the electric field (Fig. 2c). This difference is reproduced by our pres-
critical for non-adiabatically inducing a moving condensate mac- ent modelling. In addition, the 0.5 THz (red) pump pulse also has
roscopic quantum state with forbidden Anderson pseudo-spin more oscillation cycles (Fig. 2a), that is, a sharper below-resonance
modes. Figure 2 compares quantum beating spectra obtained from pump spectrum (Fig. 2b), while the 1 THz (blue) one tends to excite
coherent THz pump–THz probe dynamics driven by three different larger QP populations due to spectral overlap and proximity to the
electric-field waveforms of oscillation cycles and carrier frequency SC gap shown in Fig. 2b. Second, the single-cycle 1 THz pulse (grey,
(Fig. 2a,b) and temporal asymmetry (Fig. 2c), due to the nonlinear 47 kV cm−1) shows a significantly broadened second PSO peak
coupling effects. Specifically, to approximately evaluate the role of without other modes (Fig. 2f), which we attribute to the dephasing

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Articles
of resonantly excited QPs absent for the multi-cycle (narrowband)
0.5 THz pulse (Fig. 2b). The above comparison indicates that the
symmetry breaking and HH modes are determined by the interplay
of pulse asymmetric driving, pulse carrier frequency and oscillation
cycles. The importance of more field cycles (sharper spectral width)
and lower driving frequency (less dephasing with minimal QP exci-
tations) is consistent with our observation that the 0.5 THz pulse
driving (Fig. 2a) is the most favourable for observing the nonlinear
modes; for example, it shows a stronger second PSO peak than even
the first-order linear supercurrent peak (Fig. 2d), unlike for the
1 THz pump (Fig. 2e). Third, the sharp first-order peaks seen for 0.5
and 1 THz pumping, which underpin condensate flow and, thereby,
broken symmetry in Fig. 2d,e, are absent in both a dirty-limit NbN
sample (inset, Fig. 2e) and for the single-cycle 1 THz pump that
excites large QP populations (Fig. 2f). Finally, the simulated coher-
ent THz pump–probe responses of the current-carrying quantum
state (inset, Fig. 2d) show excellent agreement with the experimen-
tal data in Fig. 2d, which corroborates our above assignments of
the observed collective modes. We conclude that the ultrafast SC
nonlinear response results from the interplay of two different pho-
toinduced effects: lightwave nonlinear acceleration of a moving
condensate state with finite momentum pairing and dephasing via
photoexcited QP populations.
Light-induced gapless superconductivity
The non-thermal transition from gapped BCS to gapless superfluid
state driven by the multi-cycle field E1THz pumping is demonstrated
in Fig. 3a (σ1) and Fig. 3b (σ2), which show the dissipative and
inductive nonlinear responses, respectively, after Δtpp = 100 ps. The
real and imaginary parts of the conductivity measure separately the
QP excitation gap and SC order parameter (ns). σ1 reveals the partial
quench of the SC gap for low fields (E1THz = 34 kV cm (blue circles),
45 kV cm−1 (magenta circles) and 62 kV cm−1 (black circles)) and a
transition to a gapless SC state at ~78 kV cm−1 (red diamonds). The
latter corresponds to fully filling the gap in σ1, as seen by comparing
σ1(ω) with the normal state (grey line, Fig. 3a). Although the THz
QP
field quenches E min , a diverging σ2 arises from the reactive SC coher-
ence peak nsδ(ω = 0). Most intriguingly, despite the gapless conduc-
tivity demonstrated by σ1, the quench of the SC order parameter and
ns is minimal in Fig. 3b. This is clearly seen from the similar diver-
gence of the pump-induced (red diamonds) and equilibrium (black
dotted line) σ2, which indicates the observation of light-induced
gapless superconductivity. Such a gapless SC state with ns ≠ 0 can
be driven by condensate flow ps ≠ 0 and is distinct from previously
known gapless QP states, realized after strong depletion of the
condensate, ns ≈ 0. Although the condensate quenching has been
achieved previously by photoexcitation of large QP populations via
broadband single-cycle pumping7, the gapless SC state is distinct
and achieved here in a non-equilibrium supercurrent-carrying
coherent state with minimally quenched ns, driven by nonlinear
asymmetric photoexcitations via intense multi-cycle THz pulses.
The excitation spectrum of such a quasi-stationary ordered state
with finite Cooper pair velocity after 100 ps is intuitively captured
by Fig. 1b. QP excitations moving against a critical condensate flow,
vs ≈ 3.15 × 10 4 cm s−1, are energetically favourable, but only at certain
k-points. This corresponds to populating −k0 + ps↑ and −k0 + ps↓
states with QPs after removing the Cooper pairs (k0 + ps↑, −k0 + ps↓)
and (−k0 + ps↑, k0 + ps↓) from the condensate.
Non-thermal control of supercurrent-carrying states
The non-thermal dynamics of the moving condensate states can
exhibit much longer (~100 ps) rise times after the THz driving than
for a single-cycle pulse7, which, as shown in Fig. 3c, strongly depends
on the pulse temporal profile. This observation indicates a new tun-
ing method for driving non-equilibrium protected quantum states.
By comparing in Fig. 3c the ΔE/E0 dynamics excited by three different
NATurE PHoToniCS
THz pump waveforms (Fig. 2a), we demonstrate control of the
100 ps time evolution by tuning the intensity, field cycles and non-
linear asymmetry in the temporal profile of the driving THz field
pulse. We first compare the time evolution for the two multi-cycle
pulses, which are centred at 0.5 THz (red line, Fig. 3c) or 1 THz (blue
line, Fig. 3c). These two pulses induce distinctly different temporal
pathways (Fig. 3c). First, the very early regime of coherent time evo-
lution (marked as regime no. 1) displays pronounced PSOs, includ-
ing symmetry-forbidden harmonics depending on the pulse shape.
Second, we observe that the much longer temporal evolution well
after the excitation pulse is controlled by the pulse shape (marked
as regime no. 2). Third, the pulse energy required to reach a similar
non-equilibrium state after delayed timescales (marked as regime
no. 3) differs by an order of magnitude between the two multi-cycle
pulses: 12 nJ versus 130 nJ for 0.5 and 1 THz pulses, respectively.
Intriguingly, the most pronounced delayed build-up appears in the
0.5 THz pump trace (red line) with much lower pulse energy. Such
slow 100 ps dynamics coincides with the appearance of the forbid-
den Anderson pseudo-spin modes from the asymmetric multi-cycle
nonlinear THz field driving seen in Fig. 2d. These distinguishing fea-
tures clearly indicate non-thermal evolution of the discovered super-
current-carrying state with minimal SC quench. For a macroscopic
condensate flow22,23, the collective ps(t) CM momentum of many
Cooper pairs is ‘protected’, for example, against phonon scattering24,
unlike for individual QPs. In contrast, a single-cycle broadband pulse
centred at 1 THz directly excites non-equilibrium QPs by the part of
its spectrum above 2ΔSC (Fig. 2b). Such QP populations quench ns
(ref. 7), largely suppress the coherent oscillations and lead to a very
fast rise time of ~1 ps (grey line, Fig. 3c). For such a pulse spectrum,
QP generation and dephasing dominate over condensed Cooper pair
dynamics and damp the nonlinear modes (Fig. 2f). Although low-
field single-cycle pulsed excitation can also minimize the SC quench,
the post-quench states in this case still show fast subpicosecond rise
times during the pulse (inset, Fig. 3c), a strongly broadened second
PSO mode and no first-order supercurrent mode (Fig. 2f).
A careful study of the complex conductivity (σ1(ω, Δtpp), σ2(ω,
Δtpp)) in Fig. 3d,e relates the delayed rise of ΔE/E in regime no. 2
(Fig. 3c) to the filling of the QP excitation gap by additional spec-
tral weight. By comparing the non-equilibrium σ1 at 20 ps and
100 ps for our two multi-cycle pulses, we see that the initial gap
filling continues with a pronounced delayed rise for pump pulse
with ωpump = 0.5 THz (Fig. 3d). However, the slow rise becomes less
obvious for ωpump = 1 THz (Fig. 3e), consistent with the respective
ΔE/E dynamics in Fig. 3c, as a faster component emerges. This
faster dynamics dominates in the case of single-cycle 1 THz pump-
ing (grey line in Fig. 2c), as QP excitation dominates over light-
wave acceleration, also evidenced by the absence of HH peaks.
Unlike for σ1, after multi-cycle pumping well below the SC gap,
there is very little change in the condensate density ns measured
by σ2(ω) (Fig. 3d,e).
For a more quantitative analysis, we plot the QP density (q, red
circle), extracted from the integrated σ1, and the superfluid density
(p, blue circle) extracted from the σ2 divergence, as well as their sum
(Σ, black symbol), as a function of ETHz at 1 THz (inset, Fig. 3b).
It is clear that the quenched SC coherence peak nsδ(ω = 0) cannot
account for the nearly doubled Σ, for example, for ETHz = 78 kV cm−1.
The additional spectral weight during the supercurrent-carrying
state evolution is consistent with quenching of the competing
martensitic orders as discussed in ref. 21. A spectral weight trans-
fer mechanism has been also explored in ultrafast dynamics of
competing spin density wave order25–28. In addition, Fig. 3f shows
the transient complex conductivity σ1(ω,Δtpp) of the supercurrent-
carrying state at time delays Δtpp = −10–1,000 ps and 4.1 K with
E1THz = 109 kV cm−1. The gapless σ1(ω) with finite superfluid density
still persists after Δtpp = 100 ps, which again indicates a long-lived
moving condensate well after the pulse. The superfluid momentum
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NATurE PHoToniCS Articles
a b 12
Multi-cycle Spectral weight ∑
∆tpp = 100 ps
6 ω1THz –1
78 kV cm 1

σ1 (104 Ω–1 cm–1)

σ2 (104 Ω–1 cm–1)

62 kV cm–1 8
4 45 kV cm–1 q (E )/q0 p (E )/q0
34 kV cm–1 0
Static, 18 K 4 0 20 40 60 80
2 E1THz (kV cm–1)

0 Static, 4.1 K
0
2 4 6 8 10 2 4 6 8 10
ω (meV) ω (meV)

c
E0.5THz
0.4 No. 1 Single-cycle ω1THz No. 2 No. 3
=11.5 kV cm–1
Multi-cycle
E1THz
0.3 T = 4.1 K =60 kV cm–1
E1THz
∆E/E

∆tpp (ps) =122 kV cm–1

0.2 Multi-cycle ω1THz 0 2 4 6 8 10

Singe-cycle ω1THz
0.2

∆E/E
0.1 27 kv cm–1
7 kv cm–1
Multi-cycle ω0.5THz 0
0
–1 0 1 2 3 4 5 50 100 500 1,000
∆tpp (ps)
d e f
0.5 THz 1 THz
σ2 (104 Ω–1 cm–1)

12 ∆tpp = –10 ps
σ2 (104 Ω–1 cm–1)

12
Multi-cycle Multi-cycle

σ1 (ω) (104 Ω–1 cm–1)

–1 –1
3 8 11.5 kV cm 60 kV cm 9
8
Pump
4 4 6
Static, 18 K
20 ps
0 3
0
σ1 (104 Ω–1 cm–1)

1 3 5 7 9 1 3 5 7 9
2 0
ω (meV) ω (meV)
∆tpp = 20 ps ∆tpp = 20 ps
100 ps
100 ps 100 ps T = 4.1 K
250 ps 250 ps
750 ps 750 ps
1 750 ps

1,000 ps
–10 ps
–10 ps –10 ps
0
1 3 5 7 9 1 3 5 7 9 2 4 6 8 10
ω (meV) ω (meV) ω (meV)

Fig. 3 | Light-driven gapless superconductivity by non-thermal control of the supercurrent-carrying quantum states. a,b, Real (a) and imaginary (b) parts
of the THz-driven transient state conductivity spectra σ1(ω) and σ2(ω) at Δtpp = 100 ps as function of driving field, compared to the static SC state at 4.1 K
(grey solid line) and the normal state (grey dash line) at 18 K. Inset: QP density q (red circles) was extracted by integrating σ1(ω) spectral weight (SW) and
the condensate density p (blue circles) from the low-frequency divergence in σ2(ω). q0 denotes the normal state QP SW. Σ = q/q0 + p/q0 (black symbol) is
larger than its normal state value of 1, which indicates a pump-induced extra SW inside the gap. c, Temporal dynamics of ΔE/E under three different driving
fields: multi-cycle 0.5 THz (red) and 1 THz (blue) and single-cycle (grey) pump centred at 1 THz. Inset: ΔE/E dynamics driven by single-cycle THz pump at
E field 7 kV cm−1 and 27 kV cm−1. d,e, Post-driving σ1 and σ2 (insets) spectra at pump–probe delays from −10 ps to 750 ps in c for multi-cycle 0.5 THz (d) and
1 THz (e) pumping. The observed small change in σ2 indicates that ΔE originates from the large pump induced change in σ1, which arises from filling of the
QP excitation energy gap due to long-lived supercurrent flow with finite order parameter and minimal quenching of condensate density. f, Transient state
conductivity spectra σ1(ω) at Δtpp from −10 ps to 1,000 ps under multi-cycle 1 THz pump with 109 kV cm−1 peak electric field at 4.1 K.

diminishes only after long, technologically relevant, nanosecond Gauge-invariant density matrix simulations
timescales (for example, in 750 ps and 1,000 ps traces versus the To explore the pathways for nonlinear dynamics of a super-
−10 ps one (red symbols)), consistent with a persistent current with current-carrying coherent state, we solved the gauge-invariant
lifetime in the nanosecond range. density matrix nonlinear equations of motion outlined in the

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Articles NATurE PHoToniCS

a e
20 3.6 kV cm–1
8.8 kV cm–1

ETHz (kV cm–1)

10
–0.05
0

psa0
–10 16 kV cm–1 –0.10 LPS
–20 28 kV cm–1 Nonlinear
–0.15 Gauge-invariant, symmetric
b
0.4 Gauge-invariant, asymmetric
–0.20
0.2
f 1.0
p s a0

0
0.8
–0.2

(Δ0 – Δ∞)/Δ0 (%)

0.6 Regime
c 5 I II III
0.4
4
2ΔSC (meV)

3 0.2

2 0
1 g
0
d 2
Excitation energy

0
E QP (meV)

0
Excitation

–4

–2
–8

–4
–10 –5 0 5 10 15 20 0 5 10 15 20 25 30
∆tpp (ps) E THz (kV cm–1)

Fig. 4 | Gauge-invariant quantum kinetic calculation of the density matrix for the periodically driven, supercurrent-carrying macroscopic state. a, The
asymmetric THz waveform with peak E fields ranging from 3.6 to 28 kV cm−1 centred at 1 THz used in the theory simulation. b–d, Temporal dynamics of
condensate momentum psa0 (a0 is the lattice constant) (b), SC order parameter 2ΔSC (c) and excitation energy EQP (d) calculated for the THz waveform in
a. e–g, Comparison of the simulation results for psa0 (e), SC order parameter change (f) and excitation energy (g) for the state after the pulse, obtained
for the linear (black rectangle) and nonlinear (red triangle) Anderson pseudospin models, to those using full theory with symmetric (green circles) and
asymmetric (blue circles) THz pump. The latter shows excellent agreement with the experimental results and allows access to three different regimes
(marked by red arrows) by increasing the driving field: partial quench of ΔSC and EQP (regime I), the gapless SC state with ΔSC ≠ 0 and EQP = 0 (regime II) and
the gapless QP coherent state without SC (regime III).

Supplementary Information. These describe the interplay between
Anderson pseudo-spin nonlinearity and SC quantum transport
driven by lightwave acceleration. In this way, we describe the initial
condition created by coherent time evolution (few picoseconds) due
to strong coupling of electromagnetic fields and its dependence on
the driving pulse temporal profile. For this we extend previous stud-
ies of HH generation and nonlinear photocurrent coherent control
in non-superconducting systems10,29, as well as previous treatments
of quantum transport effects in SCs30,31. Here we neglect the effects
of non-thermal coupling to the martensitic order in order to focus
on the most critical elements, that is THz light-induced conden-
sate flow ps(t) and spatial modulation of SC pairing. Figure 4a
shows a slightly asymmetric sub-gap pump pulse Eeff(t) with cen-
tral ℏωpump = 4.1 meV, which drives the time-dependent superfluid
momentum ps(t) shown in Fig. 4b, corresponding to rapidly oscil-
lating Cooper pair CM momentum. The latter determines the light-
induced phase of the SC order parameter, whose amplitude ΔSC(t),
characterizing SC coherence and ns, is shown in Fig. 4c. Although
With lightwave acceleration, we find three different regimes
controlled by the pulse. For the lowest two pump fluences shown
QP
(purple and blue lines), both ΔSC and E min are finite after the pulse.
Although a gapless state is driven non-adiabatically during the pulse,
the system does not stay there for low fields. With increasing ETHz,
a transition to a gapless superfluid state, with ΔSC > 0 and EQP = 0, is
observed after the pulse (green curve), consistent with the experi-
ment. For very strong photoexcitation (pink curve), the system
reaches a gapless QP state with ΔSC = 0 and EQP = 0, where the mac-
roscopic coherence also vanishes. Figure 4e-g summarizes the three
different regimes (I–III) after the pulse, which create different initial
conditions for delayed time evolution controlled by ETHz(t). Figure 4e
plots the field dependence of the supercurrent momentum ps after
the pulse and compares the symmetric (green curve) and slightly
asymmetric (blue curve) effective pulse shapes. The acceleration of
the Cooper pairs and odd-order HH generation nonlinearities criti-
cally depend on the THz pulse shape, not just its intensity (Fig. 1f).
We also compare the field dependence of ΔSC (Fig. 4f) and E min QP

ΔSC(t) decreases with ETHz for finite ps this coherence quench is
QP
more gradual than the closing of the QP excitation energy gap E min ,
shown in Fig. 4d. This result is in qualitative agreement with the
experimental findings in Fig. 3a,b and demonstrates that the THz
sub-gap pulse can non-adiabatically drive a gapless SC quantum
phase with average ΔSC > 0 and EQP = 0 only at certain k-points.
(Fig. 4g) after the pulse between the full gauge-invariant nonlin-
ear theory with (green curve) or without (blue curve) ps(t) after the
pulse and the linearized (LPS) (black curve) or fully nonlinear (red
curve) Anderson pseudo-spin models used before. The latter assume
QP
zero momentum pairing (k↑, −k↓) and give E min = ΔSC. At high
ETHz, the fully nonlinear (red curve) pseudo-spin model predicts

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NATurE PHoToniCS
a gapless quantum state with ΔSC → 0 (red curve). Unlike in our
experiment, however, this gapless state has conductivity identical to
that of the normal state32. A symmetric pulse profile (green curves)
gives ps(t) ≠ 0 only during the pulse. This approximation produces
similar results to the nonlinear pseudospin model, but for much
smaller ETHz, that is, it displays enhanced nonlinearity. Most intrigu-
ingly, the light-induced gapless SC can be driven and controlled by
a slightly asymmetric, effective pulse shape (blue curve). The lat-
ter asymmetric shape of the effective driving pulse, treated here in
a phenomenological way, can result from propagation of electro-
magnetic fields and SC order parameter phase spatial variations,
to be discussed elsewhere. Here we obtain the required combina-
tion observed in the experiment after the pulse, ps ≠ 0, ΔSC > 0 and
QP
E min = 0, for a range of ETHz (shaded area, regime II), as marked by
QP
two red arrows, highlighting the different vanishing of E min and ΔSC
for finite ps.
Conclusion
Our findings establish lightwave acceleration of supercurrents as a
dynamical symmetry-breaking principle for the discovery of col-
lective modes and emergent macroscopic quantum phases such as
gapless superconductivity. We identify the important role of inter-
ference among various quantum pathways induced by subcycle
nonlinear photocurrents and pairing interactions that are control-
lable by phase-locked THz pulse excitations in a two-pulse pump–
probe configuration.
Online content
Any methods, additional references, Nature Research reporting
summaries, source data, statements of code and data availability and
associated accession codes are available at https://doi.org/10.1038/
s41566-019-0470-y.
Received: 25 November 2018; Accepted: 19 May 2019;
Published: xx xx xxxx
References
1. Aoki, H. et al. Nonequilibrium dynamical mean-field theory and its
applications. Rev. Mod. Phys. 86, 779–837 (2014).
2. Cea, T., Barone, P., Castellani, C. & Benfatto, L. Polarization dependence of
the third-harmonic generation in multiband superconductors. Phys. Rev. B
97, 094516 (2018).
3. Matsunaga, R. et al. Higgs amplitude mode in the BCS superconductors
Nb1 − xTixN induced by terahertz pulse excitation. Phys. Rev. Lett. 111,
057002 (2013).
4. Matsunaga, R. et al. Light-induced collective pseudospin precession
resonating with Higgs mode in a superconductor. Science 345,
1145–1149 (2014).
5. Papenkort, T., Axt, V. M. & Kuhn, T. Coherent dynamics and pump–probe
spectra of BCS superconductors. Phys. Rev. B 76, 224522 (2007).
6. Rajasekaran, S. et al. Probing optically silent superfluid stripes in cuprates.
Science 359, 575–579 (2018).
7. Yang, X. et al. Terahertz-light quantum tuning of a metastable emergent
phase hidden by superconductivity. Nat. Mater. 17, 586–591 (2018).
8. Nakamura, S. et al. Infrared activation of Higgs mode by supercurrent injection
in a superconductor NbN. Preprint at http://arxiv.org/abs/1809.10335 (2018).
9. Luo, L. et al. Ultrafast terahertz conductivity probes of topologically enhanced
surface transport driven by mid-infrared laser pulse in Bi2Se3. Nat. Commun.
10, 607 (2019).
10. Reimann, J. et al. Subcycle observation of lightwave-driven Dirac currents in
a topological surface band. Nature 562, 396–400 (2018).
11. Fausti, D. et al. Light-induced superconductivity in a stripe-ordered cuprate.
Science 331, 189–191 (2011).
12. Beck, M. et al. Transient increase of the energy gap of superconducting NbN
thin films excited by resonant narrow-band terahertz pulses. Phys. Rev. Lett.
110, 267003 (2013).
13. Giorgianni, F. et al. Leggett mode controlled by light pulses. Nat. Phys. 110,
267003 (2013).
14. Mansarta, B. et al. Coupling of a high-energy excitation to superconducting
quasiparticles in a cuprate from coherent charge fluctuation spectroscopy.
Proc. Natl Acad. Sci. USA 110, 4539–4544 (2013).
Nature Photonics | www.nature.com/naturephotonics
Articles
15. Pekker, D. & Varma, C. M. Amplitude/Higgs modes in condensed matter
physics. Annu. Rev. Condens. Matter Phys. 6, 269–297 (2015).
16. Matsunaga, R. et al. Polarization-resolved terahertz third-harmonic
generation in a single-crystal superconductor NbN: dominance of the Higgs
mode beyond the BCS approximation. Phys. Rev. B 96, 020505(R) (2017).
17. Kozlov, V. V., Rosanov, N. N., De Angelis, C. & Wabnitz, S. Generation of
unipolar pulses from nonunipolar optical pulses in a nonlinear medium.
Phys. Rev. A 84, 023818 (2011).
18. Anthore, A., Pothier, H. & Esteve, D. Density of states in a superconductor
carrying a supercurrent. Phys. Rev. Lett. 90, 127001 (2003).
19. Yuzbashyan, E. A. & Dzero, M. Dynamical vanishing of the order parameter
in a fermionic condensate. Phys. Rev. Lett. 96, 230404 (2006).
20. Luo, L. et al. Broadband terahertz generation from metamaterials. Nat.
Commun. 5, 3055 (2014).
21. Yang, X. et al. Ultrafast nonthermal terahertz electrodynamics and possible
quantum energy transfer in the Nb3Sn superconductor. Phys. Rev. B. 99,
094504 (2019).
22. Semenov, A. V., Devyatov, I. A., de Visser, P. J. & Klapwijk, T. M. Coherent
excited states in superconductors due to a microwave field. Phys. Rev. Lett.
117, 047002 (2016).
23. Moor, A., Volkov, A. F. & Efetov, K. B. Amplitude Higgs mode and
admittance in superconductors with a moving condensate. Phys. Rev. Lett.
118, 047001 (2017).
24. Hansen, E. B. Infinite conductivity of ordinary and gapless superconductors.
Physica 39, 271–292 (1968).
25. Dzero, M., Khodas, M. & Levchenko, A. Amplitude modes and dynamic
coexistence of competing orders in multicomponent superconductors. Phys.
Rev. B 91, 214505 (2015).
26. Yang, X. et al. Nonequilibrium pair breaking in Ba(Fe1 − xCox)2As2
superconductors: evidence for formation of photoinduced excitonic state.
Phys. Rev. Lett. 121, 267001 (2018).
27. Patz, A. et al. Ultrafast observation of critical nematic fluctuations and giant
magnetoelastic coupling in iron pnictides. Nat. Commun. 5, 3229 (2014).
28. Patz, A. et al. Critical speeding-up of non-equilibrium electronic relaxation
near nematic phase transition in unstrained Ba(Fe1 − xCox)2As2. Phys. Rev. B
95, 165122 (2017).
29. Langer, F. et al. Lightwave valleytronics in a monolayer of tungsten diselenide.
Nature 557, 76–80 (2018).
30. Stephen, M. J. Transport equations for superconductors. Phys. Rev. 139,
A197 (1965).
31. Yang, F. & Wu, M. W. Gauge-invariant microscopic kinetic theory of
superconductivity in response to electromagnetic fields. Phys. Rev. B 98,
094507 (2018).
32. Chou, Y. Z., Liao, Y. & Foster, M. S. Twisting Anderson pseudospins
with light: quench dynamics in terahertz-pumped BCS superconductors.
Phys. Rev. B 95, 104507 (2017).
Acknowledgements
Work at Iowa State University was supported by the Army Research Office under award no.
W911NF-15-1-0135 (THz quantum spectroscopy). Work at the University of Wisconsin
was supported by funding from the Department of Energy Office of Basic Energy Sciences
under award no. DE-FG02-06ER46327 (structural and electrical characterizations) and
Department of Energy grant no. DE-SC100387-020 (thin-film synthesis). The theory
work at the University of Alabama, Birmingham was supported by the US Department of
Energy, Office of Science, Basic Energy Sciences under award no. DE-SC0019137. The THz
spectroscopy instrument was supported in part by the W.M. Keck Foundation.
Author contributions
X.Y., C.V. and J.W. performed the experimental measurements, collected the data and
analysed the results. C.S., J.H.K. and C.B.E. designed, fabricated and characterized the
thin film heterostructures. M.M. and I.E.P. developed the theory and performed the
quantum kinetic calculations. J.W. supervised the study, and wrote the paper together
with I.E.P. and with help from all authors.
Competing interests
The authors declare no competing interests.
Additional information
Supplementary information is available for this paper at https://doi.org/10.1038/
s41566-019-0470-y.
Reprints and permissions information is available at www.nature.com/reprints.
Correspondence and requests for materials should be addressed to J.W.
Publisher’s note: Springer Nature remains neutral with regard to jurisdictional claims in
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Articles
Methods
Sample preparation. A highly textured Nb3Sn film of 20 nm thickness on 1 mm
Al2O3 (10–12) substrate was used, with a much smaller impurity scattering
rate than in previous THz studies3,4,12. Both atomic force microscopy and X-ray
diffraction characterizations indicate small r.m.s. roughness of ~4 nm and clear
diffraction peaks along the (0 1 2) direction. Grains are oriented in the (023)
direction. The static THz electrodynamics of Nb3Sn is extensively studied and
discussed in ref. 21.
Experimental details. A THz pump and THz probe spectroscopy were used;
the set-up and data acquisition scheme are described in detail in ref. 7. In the
present work, the broadband, single-cycle intense THz pulse generated from an
MgO-doped LiNbO3 nonlinear crystal was selectively tuned to narrowband, multi-
cycle oscillations by using THz filters centred at 0.5 THz (2.1 meV) and 1 THz
(4.1 meV). The full-width at half-maximum (FWHM) values of these two filters
were 0.108 THz and 0.168 THz, respectively. The FWHM beam diameters of the
narrowband 1 THz and 0.5 THz pump and the broadband 0–3 THz probe were
1.2, 2.4 and 0.8 mm, respectively. A 2-mm-diameter pinhole was located before the
studied Nb3Sn film to further ensure uniform excitation of the samples measured
by the THz probe.
∼
We experimentally determined the complex transmission texp by comparing
the transmitted THz E fields through the sample and reference with Fourier
transformation and Fresnel equations:
ref
Eout
∼ E in 1 + nsub −i 2π (d s)
texp = = ×e
( )i sin β
s
Eout n
E in
(1 + nsub)cos βs− ns + nsub s
s
where βs = 2π nsds. Ein and Eout are the incident and transmitted THz pulses,
λ0
respectively, through either substrate (ref) or sample (s). nsub and ns are the
NATurE PHoToniCS
refactive index for substrate and sample, respectively. ds is the sample thickness.
Subsequently, THz response functions such as the complex conductivity
σ∼ = σ1(ω) + iσ2(ω) were measured and used to characterize the dynamics and
spectra of the correlated electronic states, as shown in Fig. 3a,b.
Theoretical modelling. A summary of the quantum kinetic theoretical modelling
is provided in the Supplementary Information. The gauge-invariant superfluid
momentum ps(t) was induced via acceleration of the electron condensate by the
oscillating THz pulse and by the spatial dependence of the wavefunction phase,
equation (1), as determined by the equation of motion
∂tpS(R, t ) = 2∇R μeff (R, t ) + 2eE(R, t ) = 2eE eff (R, t ) (3)
where E(R,t) = −∇Rϕ(R,t) − ∂tA(R,t) is the effective time-dependent oscillating
electric field that drives the SC, determined by Maxwell’s equations with nonlinear
photocurrent sources driven by the pump (we neglect magnetic fields). ϕ is the
scalar potential. The equation
1 ∂
μeff (R, t ) = ζ(R, t ) + e ϕ(R, t ) + μ(R, t ) (4)
2 ∂t
describes the effects of spatial variations, which depend on the Coulomb and
lattice interactions and on the spatial and temporal variations of the complex-
order parameter phase. In addition, the light-driven supercurrent in our Nb3Sn
SC can be obtained intuitively using a classical circuit model with inputs from the
experimentally measured THz pulses in a nonlinear crystal, as discussed in the
λ0 (2)
Supplementary Information.
Data availability
The data that support the plots within this paper and other findings of this study
are available from the corresponding author upon reasonable request.
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