Chiral Phonon Induced Spin-Polarization J. Fransson Department of Physics and Astronomy Box 516 751 20 Uppsala University Uppsala Sweden

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Chiral Phonon Induced Spin-Polarization
J. Fransson
Department of Physics and Astronomy, Box 516, 751 20, Uppsala University, Uppsala, Sweden
(Dated: October 25, 2022)
The current understanding of chirality suggests the existence of a connection between structure and angular
momentum, including spin. This is particularly emphasised in the chiral induced spin selectivity eect, where
chiral structures act as spin filters. However, the recent discovery of chiral phonons have demonstrated that
phonons too may carry angular momentum which also can be regarded as magnetic moments which add to
the total moment. Here, it is shown that chiral phonons may induce a non-trivial spin-texture in an otherwise
non-magnetic electronic structure. By considering a set-up in which electrons and phonons are interfaced with
each other, it is shown that chiral phonons may transfer its angular momentum into the electron reservoir which,
thereby, becomes spin-polarized. It is, moreover, shown that an equivalent mechanism does not exist whenever
the electrons are interfaced with achiral phonons.
Phonons represent the collective nuclear motion within a
structure. As such, phonons are the quantum mechanically
defined quantities with which the mechanical degrees of free-
dom are eectively incorporated into the framework of the
general quantum field theory. While traditionally being re-
garded as a quantity carrying linear momentum, it is only re-
cently that angular momentum of phonons have been consid-
ered. An incomplete list of important results are phonon Hall,
phonon spin Hall, and phonon angular momentum Hall ef-
fects [17], phonon contribution to spin-relaxation processes
[811] and the Einstein-de Haas eect [10,1214], phonon-
ically mediated spin-spin interactions [15,16], temperature
gradient induced phonon angular momentum [17], and opti-
cally activated chiral phono-magnetic eects [1820]. Exper-
imentally, progress has been made in observations of chiral
phonons [2125], and phonon induced magneto-thermal prop-
erties [2628].
The existence of phonon angular momentum opens up the
possibility to couple the electronic spin-degrees of freedom
with the mechanical. It is well-established that spin and nu-
clear motion are coupled directly through, e.g., the Elliot-
Yafet mechanism [2934], but also indirectly via the elec-
tronic structure [15], and it has been demonstrated that such
coupling opens for a viable explanation of the chiral induced
spin selectivity eect [3437].
Hitherto, however, the angular momentum of phonons and
electrons have been considered as separate from one an-
other, where the magnetic moment associated with the chi-
ral phonons have been studied in its own right. While this
is definitely pertinent, the eects angular momentum trans-
fer between phonons and electrons has been discussed in a
semi-classical model [38], in which a spin-dependent cou-
pling between phonons and electrons is assumed and it is
demonstrated that chiral phonons may give rise to the spin-
Seebck eect, something that was also recently observed in
experiments [39]. Nonetheless, the mechanism that enables
the angular momentum transfer is yet to be discussed. The
purpose with this Letter is to present a coherent theory that
ties the existence of phononic angular momentum to a broken
electronic spin-degeneracy. It is shown that the mechanism is
provided through a vibronically assisted spin-orbit interaction
and while this coupling is always present, chiral phonons are
required for inducing a spin-polarization.
Chirality is a geometrical property where the structure lacks
both inversion and reflection symmetries. It is easy to demon-
strate that chiral phonons must carry a non-vanishing angular
momentum Jph. This can be seen directly from the definition
Jph(t)=ZQ(r,t)×˙
Q(r,t)dr,(1)
where Qis the nuclear displacement, which is connected
to phonons through the relation Q(r,t)=PqlqqQp(t)eiq·r,
where Qq=bqµ+b
¯
qµ, is the quantum phonon displacement
operator. Here, bqand b
qdenote the phonon destruction and
creation operators, respectively, with q=(q,µ) (¯q=(¯
q,µ)=
(q,µ)) comprising the wave vector qand normal mode µ,
and lq=p}/2ρvωqwhich defines a length scale in terms of
the phonon energy ωq, density ρ, and volume v, whereas qis
the displacement polarization vector.
The expectation value of the angular momentum, hence, as-
sumes the form
hJphi(t)=lim
t0titX
pq
lplqpׯqD>
pq(t0,t)Zei(pq)·rdr,(2)
where D>
pq(t0,t)=(i)hQp(t0)Q¯q(t)idefines the correlations
between the phonons Qp(t0) and Q¯p(t). The expression in Eq.
(2) shows that a finite phonon angular momentum requires
non-collinear polarisations pand ¯q.
Non-collinear polarizations can on the one hand be
achieved when there is a mechanism that mixes the phonon
modes pand q. Such mode mixing may originate from, e.g.,
anharmonic eects or scattering odefects acting upon the
otherwise orthogonal modes defined in the harmonic approxi-
mation.
In the harmonic approximation, the phonons can, up to
a constant, be summarised the Hamiltonian form as Hph =
Pqωqb
qbq. In this form, it is assumed that the phonon modes
do not mix which, therefore, leads to a vanishing angular mo-
mentum. However, the introduction of a component of the
kind Wqµνb
qµbqνprovides a mode mixing, which can be un-
derstood as chirality.
arXiv:2210.12722v1 [cond-mat.mes-hall] 23 Oct 2022
2
To see this, consider the phonon spinor Φq={bqµi}N
i=1, for
Nmodes, which enables us to write the phonon model as
Hph =X
q
Φ
qωqΦq.(3)
Written like this, the phonon spectrum is defined through
the matrix ωq=ω0qτ0+ω1q·τ, where ω0and ω1represent
the mode conservative and mode mixing components, respec-
tively, whereas τ0and τare the N-dimensional identity and
vector of spin matrices. While in this model it is assumed that
the mixing only takes place between modes µiand µjwith
the same momentum q, it is straight forward to generalise the
model to also include mixing between dierent momenta.
Considering a structure with two modes, such that τre-
duces to the Pauli matrices, the phonon Green function
Dq(z)=hhΦq|Φ¯
qii(z), can be written as
Dp(z)=2ωq
z2ω2
0qω2
1q+2ω0qω1q·τ
(z2ω2
0qω2
1q)24ω2
0qω2
1q
(4a)
=1
2X
s=±1
2ωqs
z2ω2
qsτ0+sˆω1q·τ,(4b)
where ωqs=ω0q+sω1q,ω1q=|ω1q|and ˆω1q=ω1q1q. The
form of this propagator written in Eq. (4b) explicitly describes
two modes with opposite helicity, or, chirality.
On the other hand, the polarization for a chiral mode is
neither reflection nor inversion symmetric, where the lat-
ter condition leads to that
qµ=¯
qµ,qµ, since equal-
ity in the last relation requires inversion symmetry. For,
e.g., a helical structure with transversal and longitudi-
nal lattice parameters aand c, respectively, the polariza-
tion may be expressed as q=(acosφq,asinφq,¢φq)/d(φq),
where ¢ =c/2πand d(φq)=qa2+¢2φ2
q, which displays
a variation of the mode that depends on the azimuthal
angle φq. Hence, for such a mode, the vector prod-
uct qׯ
q=(a¢φqsinφq,a¢φqcosφq,a2sin2φq)/d2(φq),
which suggests that a free chiral phonon mode, for which
D>
q(t,t0)=(i)[nB(ωq)eiωq(tt0)nB(ωq)eiωq(tt0)], where
nB(ω) is the Bose-Einstein distribution function, carry the
non-vanishing angular momentum
hJphi=ωql2
q
πd2(φq)
a¢φqsinφq
a¢φqcosφq
a2πsin2φq
.(5)
It is important to notice that the o-diagonal components of
the phonon propagator, Eq. (4b), carry the phase factors e±iφp,
where φpdefines the azimuthal angle of the momentum vector
p. This phase dependence reoccurs also in the helical polar-
ization vector and is an essential feature of chirality. Due to
this phase dependence, the phonons necessarily carry angular
momentum.
The objective in this Letter, is to show that the phononic
angular momentum can be transferred to the electronic sub-
system and, hence, induce a spin-polarization. For this sake,
consider the coupling between electrons and phonons, which
generally can be written as [34]
He-ph =X
kq
ψ
p+kUkqψkQq,(6)
where the coupling matrix Ukq=Ukqσ0+Jkq·σaccounts
for a spin-conservative electron-phonon coupling, Ukq, and
an electron-phonon assisted spin-orbit interaction, Jkq.
The spin-polarisation hMkiof the electrons are calculated
using the identity hMki=(i)spσRG<
kk(ω)dω/4π, where
G<
kk0(ω) defines the lesser form of the general single electron
Green function Gkk0(z)=hhψk|ψ
k0ii(z), whereas sp denotes
the trace over spin 1/2 space. To the second order (Hartree-
Fock) approximation in the electron-phonon coupling, this
Green function can be calculated from the Dyson equation
Gkk0(z)=δ(kk0)gk(z)+gk(z)X
κ
Σ(HF)
kκ(z)Gκk0(z),(7a)
Σ(HF)
kk0(z)=(i)δ(kk0)X
qq0
Dqq0UkqspZG<
kk(ω)Uk¯q0dω
2π
1
βX
zνqq0
UkqGkk0(z+zν)Uk0¯q0Dqq0(zν),(7b)
where Dqq0=Rδ(ω)Da
qq0(ω)dω.
While this equation should be self-consistently solved, for
an analysis of the induced spin symmetries, it is sucient to
replace the electronic Green functions in these expressions
with its unperturbed form gk(z)=σ0gk(z), where gk(z)=
1/(zεk) and g<
k(ω)=2πσ0f(ω)δ(ωεk), whereas f(ω) is
the Fermi-Dirac distribution function. These replacements
lead to the simplified self-energy
Σ(HF)
k(z)=2f(εk)X
qq0
δ(q)UkqDqq0Uk¯q0
1
βX
νqq0
gkq(zzν)UkqDqq0(zν)Uk¯q0.(8)
The Hartree (first) contribution is to lowest order linear in
the component Jkq·σwhich, hence, shows that the coupling
between the electrons and phonons may break time-reversal
symmetry. However, this contribution vanishes in this approx-
imation since there are no phonons at p=0. By contrast, the
exchange (second) contribution does not only open for break-
ing the time-reversal symmetry, since in general
UkpUkq=UkqUkq0+Jkq·Jkq0
+UkqJkq0+JkqUkq0+iJkq×Jkq0·σ,(9)
but it also provides a correlation between the electronic and
phononic degrees of freedom.
However, before showing that chiral phonon leads to a
breaking of the electronic spin-degeneracy, it is pertinent to
discuss the origin of the phonon induced spin-polarization and
spin-flip processes which are enabled by Jkq. For this purpose,
摘要:

ChiralPhononInducedSpin-PolarizationJ.FranssonDepartmentofPhysicsandAstronomy,Box516,75120,UppsalaUniversity,Uppsala,Sweden(Dated:October25,2022)Thecurrentunderstandingofchiralitysuggeststheexistenceofaconnectionbetweenstructureandangularmomentum,includingspin.Thisisparticularlyemphasisedinthechira...

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