Dramatic Plasmon Response to the Charge-Density-Wave Gap Development in 1T-TiSe2

2025-05-03 0 0 3.44MB 7 页 10玖币
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Dramatic Plasmon Response to the Charge-Density-Wave Gap Development in
1T-TiSe2
Zijian Lin,1, 2, Cuixiang Wang,1, 2, A. Balassis,3J. P. Echeverry,4A. S. Vasenko,5, 6 V. M. Silkin,7, 8, 9
E. V. Chulkov,7, 8, 5 Youguo Shi,1, 10 Jiandi Zhang,1Jiandong Guo,1, 2, 10, and Xuetao Zhu1, 2, 10,
1Beijing National Laboratory for Condensed Matter Physics and Institute of Physics,
Chinese Academy of Sciences, Beijing 100190, China
2School of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China
3Department of Physics and Engineering Physics, Fordham University,
441 East Fordham Road, Bronx, NY 10458, USA
4Universidad de Ibagu´e, Carrera 22 Calle 67 B, Av. Ambal´a, Ibagu´e-Tolima, Colombia
5HSE University, 101000 Moscow, Russia
6I. E. Tamm Department of Theoretical Physics, P. N. Lebedev Physical Institute,
Russian Academy of Sciences, 119991 Moscow, Russia
7Donostia International Physics Center (DIPC),
20018 San Sebasti´an/Donostia, Basque Country, Spain
8Departamento de Pol´ımeros y Materiales Avanzados: F´ısica,
Qu´ımica y Tecnolog´ıa, Facultad de Ciencias Qu´ımicas,
Universidad del Pa´ıs Vasco UPV/EHU, Apartado 1072,
20080 San Sebasti´an/Donostia, Basque Country, Spain
9IKERBASQUE, Basque Foundation for Science, 48013 Bilbao, Basque Country, Spain
10Songshan Lake Materials Laboratory, Dongguan, Guangdong 523808, China
1T-TiSe2is one of the most studied charge density wave (CDW) systems, not only because of its
peculiar properties related to the CDW transition, but also due to its status as a promising candidate
of exciton insulator signaled by the proposed plasmon softening at the CDW wave vector. Using
high-resolution electron energy loss spectroscopy, we report a systematic study of the temperature-
dependent plasmon behaviors of 1T-TiSe2. We unambiguously resolve the plasmon from phonon
modes, revealing the existence of Landau damping to the plasmon at finite momentums, which does
not support the plasmon softening picture for exciton condensation. Moreover, we discover that
the plasmon lifetime at zero momentum responds dramatically to the bandgap evolution associated
with the CDW transition. The interband transitions near the Fermi energy in the normal phase is
demonstrated serving as a strong damping channel of plasmons, while such a channel in the CDW
phase is suppressed due to the CDW gap opening, which results in the dramatic tunability of the
plasmon in semimetals or small-gap semiconductors.
In a charge density wave (CDW) material, the CDW
gap development, which is often served as the order pa-
rameter to characterize the CDW transition [1,2], can
strongly influence the emergent phenomena of the sys-
tem. 1T-TiSe2, a quasi-two-dimensional layered mate-
rial, undergoes a three-dimensional second order CDW
transition at Tc200 K with qCDW = (1/2,0,1/2) [3].
The CDW origin of 1T-TiSe2was described by several
different mechanisms [35]. One of the most-studied sce-
narios is the electron-phonon coupling [4,613], which is
the CDW origin in many quasi-two-dimensional systems
[2]. On the other hand, the CDW order in 1T-TiSe2is
proposed to be induced by the formation of the exciton
insulator (EI) [1421]. And some recent studies claimed
that the EI and the electron-phonon coupling may coop-
eratively induce the CDW transition [2227].
Understanding the the band structure evolution is es-
sential for identifying the origin of the CDW transition
[28,29]. In the normal phase above Tc[Fig. 1(a)], 1T-
TiSe2is a semiconductor with a small indirect gap [28]
(or a semimetal with a small band overlap [9]), where the
bottom of the conduction band is almost tangent to the
Fermi level EF[30,31]. Interestingly, there exists a CDW
fluctuating band above Tc[7,8,14,32,33], which may
provide a precursor of the CDW gap [34]. In the CDW
phase below Tc[Fig. 1(b)], the gap opens by the valence
band gradually shifting toward to higher binding energy,
leaving the conduction band still tangent to EFand ac-
companying with a CDW band folding [8,9,15,16,32].
Due to the coexistence of the metallic nature and CDW
gap in both the normal and CDW phases, the plasmon
provides a good window to visualizing the effect of the
CDW gap development on the electronic properties. Re-
cently, the plasmon softening at qCDW around Tcwas
proposed to serve as the signature of the EI [21]. How-
ever, a recent theoretical study attributed the seemingly
plasmon softening signal to the interband transitions [35].
In this letter, using the momentum-resolved high reso-
lution electron energy loss spectroscopy (HREELS) with
the capability of two-dimensional energy-momentum
mapping [36], we systematically measured the plasmon
behaviors in 1T-TiSe2. Our results unambiguously re-
solve the plasmon from phonon modes and demonstrate
the existence of Landau damping [3739] to the plas-
mon at finite momentums within the full temperature
range, revealing that there is no plasmon softening at
arXiv:2210.14635v1 [cond-mat.str-el] 26 Oct 2022
2
-1
0
1
Energy (eV)
(a) Normal
Direct
Gap Fluctuating
Gap Eg
Fluctuating
Band
ΓMLA
(b) CDW
CDW
Gap Eg
Folding
Band
ΓMLA
Folding
Band
FIG. 1. Schematics of the band structure in 1T-TiSe2. (a)
band structure in the normal phase. The red and blue lines
represent the valence and conduction bands, respectively. The
fluctuating band is represented by the gray shadow. The
dashed lines indicate the Fermi level. (b) band structure in
the CDW phase. Black lines represent the folding bands due
to the distortion.
qCDW. Extraordinarily, we discover that the plasmon at
zero momentum responds to the CDW transition dra-
matically, from a broad feature covering the energy of
50 150 meV to a sharp feature with the well-defined
resonant frequency at 50 meV in the low-temperature
CDW phase. Such a wide-range tunability is attributed
to the gap opening associated with the CDW transition
that suppresses the interband damping channels of the
plasmon.
Temperature-dependent HREELS results. - The mea-
surements were performed on cleaved 1T-TiSe2single-
crystalline samples in situ in a HREELS system with
reflected scattering geometry. The detailed experimen-
tal methods and sample characterizations are described
in the Supplementary Material (SM) [40]. The HREELS
data were collected with the sample temperature varying
from 35 to 300 K along the two high symmetry directions
Γ-M and Γ-K in the surface Brillouin zone (BZ). The in-
cident electron beam energy Eifrom 7 to 110 eV (110 eV
data presented in the main paper, while others in the SM
[40]) is used , with a typical energy resolution of 3 meV.
Figure 2shows the HREELS results of 1T-TiSe2at var-
ious temperatures. The temperature-dependent E-q//
mappings along Γ-M and Γ-K directions are presented in
Figs. 2(a)-(d).
In HREELS, the strong intensity distributions near the
Γ point are dominated by the dipole scattering, and the
relatively weak features away from the Γ point to the
BZ boundary correspond to the impact scattering regime
[41]. Then, it is obvious that there are two kinds of dis-
tinct energy loss features divided by the energy of 45 meV
at 300 K. The loss features higher than 45 meV, labeled
as P, are only located near the Γ point, which are pure
dipole scattering features and regarded as the plasmon
originating from the charge carrier both in the normal
and CDW phases [42,43]. The loss features lower than
45 meV exist throughout the BZ, which are typical im-
pact scattering signals from phonons [41]. To show their
dispersions more clearly, Figs. 2(e)-(h) display the second
differential images of the original spectra superimposed
to the calculated surface phonon dispersions (red lines)
using an 11-layer slab model (see the details in the SM
[40]). Overall, the calculated phonon dispersions, espe-
cially the optical phonon branches, match well with the
experimental results.
The evolution of the plasmon with temperature is il-
lustrated by a stacking plot of the loss features at the Γ
point [Fig. 2(i)]. As the temperature decreases from 300
K to Tc, the energy of the plasmon gets closer to the op-
tical phonon. When the temperature further decreases
below Tc, the energy of the plasmon slightly increases
and the linewidth of the plasmon changes dramatically.
These phenomena will be discussed later in more detail.
Compared to the previous HREELS study in Ref. [21],
our results show similar temperature-dependent plasmon
behavior at the Γ point, but surprisingly, we did not ob-
serve the plasmon softening at qCDW. In our energy-
momentum mappings at any temperature, the plasmon
only exists near the Γ point and does not disperse to the
low-energy range at the BZ boundary. In detail, Fig. 2(j)
shows dispersion behaviors of the plasmon and phonons
in the qspace along the Γ-M direction [44]. The plas-
mon decays from a sharp peak at q= 0.01 r.l.u. to a
weaker peak at q= 0.03 r.l.u. As qincreases, the plas-
mon is not a well-defined peak anymore at q= 0.10 r.l.u.
and disappears (indistinguishable from noise) beyond q
= 0.14 r.l.u. The reported energy loss signal over the
entire BZ at 17 K in Ref. [21], interpreted as a disper-
sionless plasmon, could be from diffusion scattering [41].
In our results, the delicate optical phonon dispersions
[those highlighted by the dashed-line rectangles in Fig.
2], which were not observed in Ref. [21], can be clearly
resolved from the plasmon. The energy range of these
optical phonon branches are close to the claimed soften-
ing plasmon energy, so the softening plasmon dispersion
around Tc[21] seems from the envelope of phonon sig-
nals. Details of the comparison are described in the SM
[40].
Landau damping of the plasmon. - The observed
plasmon damping behaviors can be well understood by
the calculations of the loss functions, which were car-
ried in the framework of time-dependent density func-
tional theory (see details in the SM [40]). For simplicity,
the calculated band structure in the CDW phase does
not include the effects of band folding and renormaliza-
tion. The calculated single particle excitation (SPE) re-
gions for the normal and CDW band structures are in-
dicated by white dashed line and shadow areas centered
at thick white dashed lines in Fig. 3, and plasmon dis-
persions are represented by color mappings of the calcu-
lated loss functions. At the lowest q, plasmons are almost
delta functions. However, plasmons broaden and weaken
rapidly approaching SPE borders. Beyond the calculated
qc= 0.024 r.l.u. [45], plasmons are not well-defined col-
lective excitations anymore due to the strong decay to
SPEs. This explains the experimentally observed fast
摘要:

DramaticPlasmonResponsetotheCharge-Density-WaveGapDevelopmentin1T-TiSe2ZijianLin,1,2,CuixiangWang,1,2,A.Balassis,3J.P.Echeverry,4A.S.Vasenko,5,6V.M.Silkin,7,8,9E.V.Chulkov,7,8,5YouguoShi,1,10JiandiZhang,1JiandongGuo,1,2,10,yandXuetaoZhu1,2,10,z1BeijingNationalLaboratoryforCondensedMatterPhysicsand...

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