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P H Y S I C S copyright © 2025 the 
Authors, some rights 
Chiral- induced unidirectional spin-t o-c harge conversion reserved; exclusive 
licensee American 
Ashish Moharana1, Yael Kapon2,3, Fabian Kammerbauer1, David Anthofer1, Shira Yochelis2,3,  Association for the 
3,4 3,4 Advancement of Hadar Shema , Elad Gross , Mathias Kläui1, Yossi Paltiel2,3, Angela Wittmann1* Science. no claim to 
original U.S. 
The observation of spin- dependent transmission of electrons through chiral molecules has led to the discovery of Government Works. 
chiral- induced spin selectivity (CISS). The remarkably high efficiency of the spin polarizing effect has recently distributed under a 
gained substantial interest due to the high potential for future sustainable hybrid chiral molecule magnetic ap- creative commons 
plications. However, the fundamental mechanisms underlying the chiral- induced phenomena remain to be un- Attribution license 4.0 
derstood fully. In this work, we explore the impact of chirality on spin angular momentum in hybrid metal/chiral (cc BY). 
molecule thin-fi lm heterostructures. For this, we inject a pure spin current via spin pumping and investigate the 
spin- to-c harge conversion at the hybrid chiral interface. Notably, we observe a chiral-i nduced unidirectionality in 
the conversion. Furthermore, angle- dependent measurements reveal that the spin selectivity is maximum when 
the spin angular momentum is aligned with the molecular chiral axis. Our findings validate the central role of spin 
angular momentum for the CISS effect, paving the path toward three- dimensional functionalization of hybrid 
molecule- metal devices via chirality.
INTRODUCTION mechanisms. Studies have demonstrated that SOC originating from 
The spin-d ependent charge transport through chiral molecules gives the helical structure of chiral molecules plays a pivotal role in the 
rise to a well-e stablished phenomenon known as chiral- induced CISS effect (20, 21). However, the magnitude of the SOC within 
spin selectivity (CISS). Over the past decade, studies have consis- these molecules is often too small to account for the substantial 
tently demonstrated chiral- induced spin polarization with efficien- spin- filtering effect observed in experiments. To address this chal-
cies of up to more than 70% (1–5). Extensive investigations into the lenge, several studies have focused on the role of SOC at the hy-
CISS effect have so far primarily focused on chiral- induced non- brid interface between heavy metals and chiral molecules. These 
equilibrium spin polarization in photoemission spectroscopy and studies have shown that CISS is a result of the interaction between 
transport measurements. The initial observation of spin-p olarized the high SOC of the metal electrode and charge distribution at the 
photoelectron emission through a polyalanine layer revealed a de- interface of the molecule and metal (22–31). Several reports have 
pendence on the chirality of the peptide molecules (6). Another ap- attempted to provide a theoretical description of chiral structures 
proach to exploring the CISS effect has involved local transport by incorporating electron- phonon and electron- electron interac-
measurements (7–11). tions. These interactions are a result of the SOC, leading to the 
However, in addition to the CISS effect in the transport of charge exchange splitting of the spin channels within the structure, ulti-
carriers, it is crucial to note that chiral molecules can also substan- mately contributing to the phenomenon of spin filtering (31, 32). 
tially affect the properties of underlying metal thin films via the CISS On the other hand, recent studies have shown that the CISS effect 
effect resulting in an equilibrium, respectively spontaneous spin po- can result from the chiral-i nduced orbital polarization effect of 
larization. The hybrid interface between molecules and metal thin chiral molecules. In this framework, the topological electronic 
films has been a fruitful playground for engineering interfacial prop- property of chiral molecules is characterized by the locking of spin 
erties through molecular design (12,  13). Hybridization between and orbital angular momentum. Electrons with orbital angular 
molecules and metal thin films leads to changes in the electronic and momentum compatible with the molecular chirality find it easier 
magnetic properties at the hybrid interface (14–19). Along with the to enter the chiral layer. This orbital polarization effect induces 
widely studied effects of charge transfer and exchange coupling at spin polarization mediated by the SOC in the heavy metal contact 
hybrid interfaces, hybridization also affects the effective spin- orbit resulting in spin selectivity in the hybrid chiral molecule metal 
coupling (SOC) in the hybrid system. Prominent examples of the system (33–35).
CISS effect upon hybridization is the emergence of a thermally driv- While these experimental studies imply that SOC plays a crucial 
en spontaneous spin polarization (18), magnetization- dependent role, conclusive evidence has so far been lacking for a pronounced 
adsorption of chiral molecules (10), and manipulation of magnetiza- impact of the adsorption of chiral molecules on the SOC in the un-
tion when chiral molecules are adsorbed on metallic and ferromag- derlying metal thin films. In this work, we demonstrate the impact 
netic surfaces (17). of chiral molecules on the inverse spin Hall effect (ISHE), which 
Numerous experimental and theoretical efforts have tried to originates from a collection of relativistic SOC phenomena (36). For 
understand the underlying microscopic origins of the CISS effect. this, we inject a pure spin current generated by ferromagnetic reso-
However, a fundamental debate persists in elucidating its microscopic nance in a ferromagnetic insulator into a hybrid metal/chiral mole-
cule bilayer. The SOC of the hybrid layer converts the spin current 
1institute of Physics, Johannes Gutenberg University Mainz, Mainz 55128, Germany. into an electromotive force via the ISHE, measurable as a voltage 
2institute of Applied Physics, the hebrew University of Jerusalem, Jerusalem signal across the metal layer (37). The results show a chirality and 
9190401, israel. 3center for nanoscience and nanotechnology, the hebrew Univer- spin polarization–dependent unidirectional ISHE in the hybrid chi-
sity of Jerusalem, Jerusalem 9190401, israel. 4institute of chemistry, the hebrew 
University of Jerusalem, Jerusalem 9190401, israel. ral system confirming that SOC and spin angular momentum play a 
*corresponding author. email: a.w ittmann@ uni- mainz. de pivotal role in this CISS effect.
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RESULTS AND DISCUSSION a self- assembled monolayer of 36-L  α-h elix polyalanine was ad-
In this study, we perform spin pumping experiments in ferrimag- sorbed on the YIG/Au sample (see schematic inset in Fig. 1C). 
netic insulator (Y3Fe5O12, YIG, 103 nm)/heavy metal (Au, 4 nm) bi- Figure 1C shows the ISHE voltage VISHE of the hybrid chiral device 
layer structures to generate a pure spin current in a nonmagnetic around ferromagnetic resonance for positive (light red) and negative 
metal layer. The samples are placed on a grounded coplanar wave- (dark red) magnetic fields along 60°. In stark contrast to the bare 
guide to excite the precession of the magnetization with an ac micro- YIG/Au device, there is a significant change in the magnitude of 
wave magnetic field (10 GHz). At ferromagnetic resonance, spin VISHE when the polarity of the magnetic field is reversed in the hy-
angular momentum is injected from the magnetic layer into the ad- brid chiral device. To probe the role of the chirality on the observed 
jacent nonmagnetic layer (38). Because of the ISHE, the resulting spin selectivity, we investigated a hybrid homochiral device with chi-
pure spin current generates an electromotive force perpendicular to ral molecules of the opposite handedness. Figure 1D shows also a 
the spin polarization and the spin current direction that can be de- significant difference in VISHE in the hybrid chiral YIG/Au/36- D α- 
tected as a voltage signal VISHE. The direction of the spin polarization helix polyalanine device between ferromagnetic resonance in posi-
in the pure spin current can be controlled by changing the orienta- tive (light green) and negative (dark green) magnetic fields along 
tion of the magnetization of the ferrimagnet using an external mag- 60°. However, the sign of the difference in VISHE is reversed between 
netic field (see the Supplementary Materials). A schematic illustration the two opposite chiralities of the molecules. This implies that the 
of the geometry of the spin pumping measurement is shown in Fig. spin selectivity in the spin-t o- charge conversion efficiency for a giv-
1A. Figure 1B shows the characteristic Lorentzian resonance shape en spin polarization direction depends on the chirality of the hybrid 
of the ISHE voltage VISHE signal around the ferromagnetic resonance chiral system. Furthermore, to disentangle the effect of the chirality 
as a function of the applied magnetic field. Here, the magnetic field of the molecules from the common chirality- independent hybrid-
was applied at an angle of 60° (+B) and 240° (−B) (Fig. 1B). As ex- ization effects of molecules on metal surfaces, we have performed a 
pected from the symmetry of the ISHE, there is no significant differ- control experiment on a hybrid system with a racemic mixture of the 
ence in the absolute magnitude of VISHE at ferromagnetic resonance polyalanine molecules and achiral molecules (see the Supplementa-
in YIG/Au between the positive (light gray) and negative (dark gray) ry Materials). The racemic mixture consists of equal fractions of 
external magnetic field. Furthermore, we note that the voltage signal both optical rotations. The ISHE voltage VISHE for the device with 
VISHE reverses its sign when the polarity of the magnetic field is in- the racemic mixture is shown in Fig. 1E. Akin to the bare YIG/Au 
verted (see the Supplementary Materials). However, to compare the sample, the magnitude of VISHE at ferromagnetic resonance does not 
absolute magnitude in the ISHE between positive and negative mag- depend on the polarity of the magnetic field. Consequently, the ob-
netic fields, the data are shown in absolute values. served asymmetry in the spin- to- charge conversion efficiency in the 
hybrid chiral system is directly linked to the chirality of the mole-
Hybrid chiral systems cules, presenting a distinct signature of the CISS effect. The depen-
To probe and quantify the impact of the CISS effect on the spin-t o- dence of the magnitude of VISHE on the polarity of the spin 
charge conversion in the hybrid heavy- metal/chiral molecule system, polarization in the pure spin current implies that the chirality of the 
Fig. 1. Inverse spin Hall effect voltage at ferromagnetic resonance. (A) Schematic representation of spin pumping at the hybrid interface between Au and chiral mol-
ecules and detection of pure spin current via the iShe by measuring the dc voltage across the Au layer. (B) iShe voltage ViShe measurement across ferromagnetic reso-
nance with spin polarization at an angle of α = 60°. the absolute magnitude of iShe for both positive and negative magnetic fields without molecules. (C) ViShe of the 
hybrid homochiral device with 36-l  α-h elix polyalanine molecules for both positive and negative magnetic fields. (D) ViShe of the hybrid homochiral device with 36-d  α- 
helix polyalanine molecules for positive and negative magnetic fields. (E) ViShe for an achiral hybrid device with a racemic mixture of polyalanine molecules for positive 
and negative magnetic fields.
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molecules substantially affects the effective SOC at the hybrid chiral the spin selectivity in the homochiral devices sharply increases at 
interface. This result is consistent with the theoretical prediction of |α| = 60° to a plateau and abruptly decreases again at |α| = 120°. In 
chiral charge transfer at the hybrid heavy metal- molecule interface self-a ssembled monolayers, the polyalanine molecules do not arrange 
resulting in a chiral charge distribution in metals (39). perfectly perpendicular to the sample surface but have been shown to 
tilt to approximately 60° with respect to the sample surface (25, 40, 41). 
Angle- dependent measurements This has been confirmed in the surface characterization of the hybrid 
In the next step, we examine the full out-o f-p lane angle dependence devices investigated in this work (see the Supplementary Materials). 
of the ISHE signal to investigate the symmetry of the spin selectivity Given this fixed out-o f- plane tilt angle, the azimuthal orientation of 
in more detail. To maximize the detected voltage signal VISHE, we the tilted molecules within the plane is distributed isotropically. Areas 
focus on the angle dependence within the plane of rotation perpen- with parallel orientation of the tilted molecules form micrometer- 
dicular to the voltage leads as shown schematically in Fig. 2A. Figure sized domains. The ISHE measurement probes the signal averaged 
2B shows the angle dependence of VISHE of the bare YIG/Au device over many domains with different azimuthal angles as depicted sche-
as a function of the out-o f-p lane angle α of the external magnetic matically in Fig. 3B. As a result, the agreement between the strong and 
field for positive and negative polarity (light and dark gray, respec- nonuniform angle dependence of the efficiency of the chiral- induced 
tively). As expected from the symmetry of the ISHE, the experimen- effect with the overall orientation of the molecules implies that the 
tal data fit well to a cos(α) function (solid line). A similar angle observed effect is vectorial. This is akin to previous reports of vecto-
dependence of VISHE is also observed for the hybrid achiral devices rial spin filtering via the CISS effect in charge currents (42).
(see the Supplementary Materials). In contrast to this, the angle- Averaging over all homochiral devices investigated in this work, 
dependent voltage signal VISHE in the hybrid homochiral devices we find a mean spin selectivity of 35 ± 8% within the angle range of 
shows a significant asymmetry between the positive and negative 60° < |α| < 120°. This magnitude of the maximum spin selectivity 
(light and dark red, respectively) external magnetic field which re- agrees well with previous reports of the CISS effect in charge current 
verses with opposite polarity of the magnetic field as shown in Fig. transport in the literature (43, 44).
2C for L-3 6 α- helix polyalanine. We emphasize that in all devices, So far, most theoretical frameworks of the CISS effect have focused 
VISHE vanishes around α = ±90° due to the fundamental symmetry on magnetoresistance in two- terminal devices. In this geometry, no 
of the ISHE. The asymmetry in the angle dependence of the ISHE in chirality- dependent magnetoresistance would be expected in the lin-
homochiral systems further confirms the presence of a chiral- ear transport regime from fundamental symmetry considerations 
induced unidirectional component in the spin- to-c harge conversion. (45, 46). In contrast, theoretical work has predicted chirality- dependent 
We can quantify the effective spin selectivity S spin- to-c harge conversion in a multiterminal device when a pure spin 
 current is injected into a chiral film (47). Our work considers similar 
|
|V (+B)
|
| −
| |
ISHE |V −BISHE( )| three- terminal devices, where a pure spin current is injected along the 
S =
|V (+B)| + |V (−B)| out-o f- plane direction and the resulting ISHE voltage is detected be-| ISHE | | ISHE | tween two transverse voltage probes. Here, the spin- to- charge conver-
Figure 3A shows the angle dependence of the extracted spin selec- sion is modulated via a quasi-e quilibrium spin polarization at the 
tivity of the L and D rotations of the hybrid homochiral and the hy- hybrid interface between the chiral molecules on the gold thin films 
brid achiral system with the racemic mixture. The hybrid achiral (18, 28). Furthermore, the angle dependence implies that in this ex-
system (blue) does not show any significant spin selectivity at any periment, the induced spin polarization direction is given by the orien-
angle. In contrast, the L and D rotations of the hybrid homochiral tation of the chiral molecules in the hybrid system rather than the 
systems (red and green, respectively) show a sizeable spin selectivity external magnetic field. The experimental results confirm that chiral 
of up to 60%. The sign of the spin selectivity is reversed for the two molecules induce chirality- dependent spin-t o- charge conversion re-
opposite helicities of the L and D polyalanine molecules. We note that sulting in a unidirectional ISHE.
Fig. 2. Angle dependence of the ISHE measurements. (A) Schematic representation of the plane of measurement where H represents the applied field, and α denotes 
the angle of the magnetic field with respect to the sample. Angle dependence of the iShe voltage for (B) a bare YiG/Au device and (C) a hybrid chiral YiG/Au/36- l α-h elix 
polyalanine device. For illustration purposes, the sign of the iShe voltage signal measured with positive magnetic field has been inverted. the solid lines show the fits to 
the experimental data points.
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Fig. 3. Angle dependence of the spin selectivity effect. (A) Spin selectivity effect represents the change in ViShe for different spin orientations for both positive and 
negative magnetic fields normalized for ViShe for l (red) and d (green) rotations of 36 α-h elix polyalanine and the racemic mixture (blue) on Au. the solid line represents a 
cubic spline interpolation. (B) Schematic depicting the orientation of domains with different azimuthal angles of the tilted molecules on Au, where the molecules are ar-
ranged at an angle of 60° with respect to the sample surface.
In summary, we have performed spin-p umping experiments to Sample fabrication process
probe the impact of chirality on pure spin currents. Our findings In the fabrication of the YIG/Au sample used in this study, a 4- nm- 
show clear signatures of the CISS effect in the spin-t o-c harge con- thick layer of gold (Au) was sputter- deposited onto YIG substrates 
version at the metal-m olecule hybrid interface. In particular, we re- with a thickness of 103 nm, grown using the liquid phase epitaxy 
port a chiral-d ependent strongly unidirectional ISHE. Through technique. The sputter deposition of the Au layer was carried out in 
angle- dependent magnetic field measurements, we verify that the an argon (Ar) plasma at a controlled rate of 0.9 Å/s with a base pres-
maximum spin selectivity efficiency occurs when the spin orienta- sure of 5 × 10−8 mbar. Standard photolithography and Ar ion etch-
tion aligns with the orientation of the molecular chiral axis. Thus, ing were used to fabricate the 100-μ m- wide and 800-μ m- long bar 
the chiral-i nduced anisotropy in the interfacial SOC acts vectorially structures. A metallic shadow mask was used to deposit Au elec-
along the axis of the chiral molecules. The CISS effect enhances and trodes. Sputtering was used to deposit 5 nm of Cr and 50 nm of Au 
reduces the spin-t o- charge conversion when the spin polarization is electrodes.
parallel and antiparallel to the chiral axis, respectively. These results 
imply that the CISS effect depends fundamentally on the electrons’ Measurement procedure
spin angular momentum and directly affects the SOC in the metal The YIG/Au sample was mounted on top of a strip line of the 
thin film. These insights open up a pathway toward targeted vecto- grounded coplanar waveguide. The input microwave power re-
rial manipulation of hybrid spintronic devices via chirality. mained consistently fixed at 10 dBm, and the microwave frequency 
was set to 10 GHz. The ferromagnetic resonance and ISHE measure-
ments were carried out using a lock- in technique modulating the 
MATERIALS AND METHODS amplitude of the microwave signal at a modulation frequency of 
The 36-L /D α- helix polyalanine (L/D-A HPA) [[H] CAAAAKAAA- 1.5 kHz. We have verified that the amplitude of the microwave ab-
AKAAAAKAAAAKAAAAKAAAAKAAAAK-[ OH]] molecules (C sorption at ferromagnetic resonance is comparable for both polari-
stands for cysteine, A for alanine, and K for lysine) were manufac- ties of the magnetic field (see the Supplementary Materials). The 
tured by Sigma- Aldrich. A 1 mM solution was prepared in absolute experiments have been performed on two samples each for both en-
ethanol and used in the experiments. The racemic mixture was pro- antiomers and the racemic mixture. The angle- dependent ISHE volt-
duced by mixing equal parts of the L and D solutions. age measurements have been performed on all devices before the 
adsorption of molecules to verify that the ISHE response is fully an-
Monolayer adsorption tisymmetric between the positive and negative polarity of the exter-
Sample cleaning was performed with boiling acetone for 10 min fol- nal magnetic field as previously reported and expected for YIG/Au 
lowed by boiling isopropanol for 10 min and subsequently double dis- bilayer samples. After the adsorption of the molecules on the YIG/
tilled water. To prepare the exposed Au surface for adsorption, it was Au devices, the full angle dependence of the ISHE voltage measure-
immersed in ethanol for 20 min to reduce the produced oxides. After- ment was repeated.
ward, the molecules were chemically adsorbed through their thiol 
head group onto the surface via a 72-h our immersion, for a dense and 
organized monolayer, in a 1 mM solution of the molecules in absolute 
ethanol in a nitrogen environment. The substrates were washed in dry Supplementary Materials
ethanol and dried off. X- ray photoelectron spectroscopy (XPS) and This PDF file includes:
Supplementary text
polarization modulation- infrared reflection- adsorption spectroscopy Figs. S1 to S13
measurements were performed to characterize the monolayer growth tables S1 to S3
(see the Supplementary Materials). References
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charge-o rdered α-h elical polypeptide monolayers on Au (111). J. Phys. Chem. C 124, (hYMMS P2022-0 3-0 44). A.M., F.K., M.K., and A.W. thank the German Research Foundation (SFB 
5734–5739 (2020). tRR 173 Spin+X 268565370 projects A01, B02, and B14). Y.K., S.Y., and Y.P. acknowledge 
Moharana et al., Sci. Adv. 11, eado4285 (2025)     1 January 2025 5 of 6
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S c i e n c e  A d v A n c e S  |  R e S e A R c h  A R t i c l e
funding from the Ministry of Science (MOS) israel. Author contributions: A.W., Y.P., and M.K. present in the paper and/or the Supplementary Materials. the raw data and the data 
conceived the study. A.M., d.A., and F.K. fabricated the samples. Y.K. and S.Y. absorbed the represented in the figures are available at https://doi.org/10.5281/zenodo.10555404.
polyalanine molecules on the sample and performed the surface characterization with help 
from h.S. and e.G. A.M. performed the ferromagnetic resonance experiments and analyzed the Submitted 1 February 2024 
data with input from A.W. A.M. and A.W. wrote the manuscript with comments and input from Accepted 25 november 2024 
all authors. Competing interests: the authors declare that they have no competing interests. Published 1 January 2025 
Data and materials availability: All data needed to evaluate the conclusions in the paper are 10.1126/sciadv.ado4285
Moharana et al., Sci. Adv. 11, eado4285 (2025)     1 January 2025 6 of 6
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