SPIXY

Spintronics and Epitaxy

Leader: L Michez

Introduction

Spintronics and Epitaxy

Our research activities are focused on the development of thin film materials and nanostructures based on metals, silicon and germanium, the most widely used semiconductor materials in electronics.

Our objective is to study the original physical properties of these objects and their integration into current electronic devices. We are particularly interested in materials and heterostructures for spin electronics -spintronics-, a branch of electronics exploiting the phenomena related to the electron spin.

Original effects related to spin-dependent electronic transport can indeed emerge from:

  • the reduction of materials to the nanometer scale,
  • the association of materials in a heterostructure.

The interfaces often play a key role in these structures. Thus, our activity is mainly oriented toward the study of heteroepitaxy, structural and chemical characterizations of nanostructures and existing interfaces, and the study of physical properties, particularly electrical and magnetic ones. Our main goal is to study the interplay between structure and physical properties.

The elaboration and growth of materials are mainly carried out using molecular beam epitaxy (MBE), a technique in which kinetic and thermodynamic aspects, epitaxial growth modes, and stress states in the films must be considered. The main used characterization techniques are RHEED (in situ monitoring of vacuum deposits), XRD, TEM, AFM, SQUID, VSM, etc.

(click to enlarge) MBE cluster

The associated research topics are:

Mn5Ge3

The development of suitable materials for spin-polarized injection into group IV semiconductors is a key step towards the full integration of spintronic devices into semiconductor technology. This approach presents itself as the most promising alternative to Si or Ge based dilute magnetic semiconductors (DMS) whose Curie temperatures (TC) remain well below 300K.

We have shown that the ferromagnetic intermetallic (FM) alloy Mn5Ge3 can be epitaxially synthesized directly on Ge(111) with a low dislocation density (10^4cm-2, cf. figure 1). The efficiency of spin-polarized current injection by tunneling through the Schottky barrier formed at the interface between a ferromagnetic metal and a semiconductor relies on a very high crystal quality of the heterostructure and an abrupt interface. We have therefore developed different growth techniques (diffusive and non-diffusive) to synthesize by molecular beam epitaxy (MBE) the Mn5Ge3/Ge heterostructure. The study of the structural properties by RHEED, DRX, TEM and AFM reveals an excellent crystal quality and an abrupt interface at the atomic scale, making this system suitable for electrical injection.

The limited Curie temperature of Mn5Ge3 (296 K) is a hindrance to its use in devices. We have shown that the incorporation of a small amount of C allows maintaining the ferromagnetic order up to 430 K. The results of our experimental studies show for the first time that C atoms are located in the octahedral sites of the Mn5Ge3 lattice as shown in Figure 2.

By complementary magnetic characterizations (SQUID, VSM, FMR, NMR, MFM...) and micromagnetism studies by OOMMF, we have shown that this material exhibits a moderate uniaxial anisotropy leading to the presence of a critical thickness above which the film structures into ribbon-like magnetic domains with out-of-plane magnetization (figure 3).

We have determined the height and width of the Schottky barrier and shown that these values can be modulated by δ-doping of Ge near the Mn5Ge3/Ge interface. Based on these results, we are working with AIST (Tsukuba, Japan) to perform spin-polarized injection into Ge in lateral structures and vertical spin gates.

Matériaux 2D 5
Fig. 1 :Mn5Ge3 thin film grown epitaxially on Ge(111) substrate.
stem

Fig.2: (a) Planar STEM image of a C dpoed Mn5Ge3 layer. Inset: unit cell of the Mn5Ge3 hexagonal lattice along the c axis. The C atom is in the octaedric interstitial site created by the type II Mn atoms.
(b), (c) et (d) Elemental map recorded by EELS showing the positions of the Mn, Ge and C atoms.
MFM

Fig. 3 :MFM image of 50 nm thick Mn5Ge3C0.5 film showing the magnetic domains structure.

Mn5Si3

Antiferromagnetic (AF) materials are magnetic at the atomic scale and non-magnetic at the macroscopic scale. This results in robustness to stray magnetic fields and an absence of leakage fields which, in addition to a fast dynamic range (in the THz range), makes them unique for solving important problems in today's ICT field (information storage, cybersecurity, device operation speed... ).

Among them, the compound Mn5Si3 is particularly interesting because it exhibits a metamagnetic phase transition between two chiral-ordered spin structures below 65K and collinear above (figure 4). Remarkably, its isostructural equivalent Mn5Si3Cx is ferromagnetic. The Mn5Si3Cx compound thus presents itself as a model structure for identifying and exploiting new transport mechanisms in complex antiferromagnetic (AF) materials.

MFM

Fig. 4: Mn5Si3 is an anti-ferromagnetic materials exhibiting an anti-colinear and a colinear phases.

DMS and quantum dots

Diluted semiconductors (DMS) obtained by incorporating a magnetic element in the semiconductor matrix would allow to combine storage and manipulation of information in the current microelectronic processes. We are particularly interested in the growth and magnetic properties of Ge and Mn based DMS.

The first growth steps of Mn on Ge(001) have shown the presence of preferred adsorption sites for Mn atoms that react with Ge to form an alloy (see figure 5) and a very strong surface diffusion, even for temperatures as low as 80°C. These results corroborate the numerous studies reporting the difficulty of obtaining Ge(1-x)Mnx DMS thin films by co-depositing Mn and Ge on Ge(001). The Curie temperatures (TC) remain limited by the low solubility of Mn in Ge (TC < 150K) for a maximum concentration of 2-3% Mn in the thin films).

first_stage_Mn-Ge_growth

Fig. 5: First growth step of Mn on Ge(001): islands are formed between the Ge dimers by consumming the Ge atoms of the adjacents rows.

Hybride organic/inorganic interfaces

Hybrid organic/inorganic interfaces could pave the way for new chemically designed multifunctional electronic devices, especially in the field of spintronics where, for example, the interfacial spin polarization can be tuned by chemical interactions and surface modifications. In this pioneering work, we have studied the formation of self-assembled monolayers on the surface of Mn5Ge3. The first steps have thus shown the feasibility of the functionalization of the Mn5Ge3 surface by octanethiol molecules (Figure 6).

Mn5Ge3_OT

Fig. 6 :functionalization of the Mn5Ge3 surface by an octanethiol SAM.

Publications

2025

Intrinsic Magnetism and Field‐Driven Spin Alignment in NiI2 Revealed by X‐ray Magnetic Spectroscopy

Ethan L Arnold, Emily Heppell, Rabindra Basnet, Binshuo Zhang, Jieyi Liu, Javier Herrero-Martín, Charles Guillemard, Yanfeng Guo, Jin Hu, Dirk Backes, Gerrit van der Laan, Thorsten Hesjedal

physica status solidi (RRL) - Rapid Research Letters (pss RRL) (2025)10.1002/pssr.202500130

Even-in-magnetic-field part of transverse resistivity as a probe of magnetic order

Antonin Badura, Dominik Kriegner, Eva Schmoranzerová, Karel Výborný, Miina Leiviskä, Rafael Lopes Seeger, Vincent Baltz, Daniel Scheffler, Sebastian Beckert, Ismaila Kounta, Lisa Michez, Libor Šmejkal, Jairo Sinova, Sebastian Goennenwein, Jakub Železný, Helena Reichlová

Applied Physics Letters 126:172404 (2025)10.1063/5.0269699

Detecting slow magnetization relaxation via magnetotransport measurements based on the current-reversal method

Sebastian Beckert, Richard Schlitz, Gregor Skobjin, Antonin Badura, Miina Leiviskä, Dominik Kriegner, Daniel Scheffler, Giacomo Sala, Kamil Olejník, Lisa Michez, Vincent Baltz, Andy Thomas, Helena Reichlová, Sebastian Goennenwein

Physical Review B 111:014441 (2025)10.1103/PhysRevB.111.014441

Unusually High Occupation of Co 3d State in Magnetic Weyl Semimetal Co 3 Sn 2 S 2

Jieyi Liu, Yiheng Yang, Jianlei Shen, Defa Liu, Gohil Singh Thakur, Charles Guillemard, Alevtina Smekhova, Houke Chen, Deepnarayan Biswas, Manuel Valvidares, Enke Liu, Claudia Felser, Tien-Lin Lee, Thorsten Hesjedal, Yulin Chen, Gerrit van der Laan

ACS Nano (2025)10.1021/acsnano.4c13750

2024

Magnetic interactions in epitaxial films of Mn5(Ge1-xSix)3/Ge(111) : 55Mn NMR study

R. Kalvig, E. Jędryka, S. Kang, M. Petit, L. Michez, M. Wójcik

Journal of Magnetism and Magnetic Materials 600:172120 (2024)10.1016/j.jmmm.2024.172120

Epitaxial growth and magnetic properties of Mn5(SixGe1-x)3 thin films

Sueyeong Kang, Matthieu Petit, Vasile Heresanu, Alexandre Altié, Thomas Beaujard, Ganaël Bon, Oscar Cespedes, Brian Hickey, Lisa Michez

Thin Solid Films 797:140338 (2024)10.1016/j.tsf.2024.140338

Anisotropy of the anomalous Hall effect in thin films of the altermagnet candidate Mn5Si3

Miina Leiviskä, Javier Rial, Antonín Badura, Rafael Lopes Seeger, Ismaïla Kounta, Sebastian Beckert, Dominik Kriegner, Isabelle Joumard, Eva Schmoranzerová, Jairo Sinova, Olena Gomonay, Andy Thomas, Sebastian Goennenwein, Helena Reichlová, Libor Šmejkal, Lisa Michez, Tomáš Jungwirth, Vincent Baltz

Physical Review B 109:224430 (2024)10.1103/PhysRevB.109.224430

Realization of Fully High‐Spin State and Strong Ferromagnetism in LaCoO3 Monolayer

Junhua Liu, Liang Si, Qinghua Zhang, Xiao Wang, Jessica Freese, Grant Harris, Mei Wu, Xinxin Zhang, Ting Lin, Ronny Sutarto, Javier Herrero-Martín, Charles Guillemard, Manuel Valvidares, Lin Li, Xiaofei Gao, Yaoyao Ji, Zhixiong Deng, Yuhao Hong, Long Wei, Yulin Gan, Lingfei Wang, Guanglei Cheng, Peng Gao, Lin Gu, Jiandi Zhang, Zhiwei Hu, Liu Hao Tjeng, Robert Green, Kai Chen, Zhaoliang Liao

Advanced Functional Materials (2024)10.1002/adfm.202401859

Observation of a spontaneous anomalous Hall response in the Mn5Si3 d-wave altermagnet candidate

Helena Reichlová, Rafael Lopes Seeger, Rafael González-Hernández, Ismaila Kounta, Richard Schlitz, Dominik Kriegner, Philipp Ritzinger, Michaela Lammel, Miina Leiviskä, Anna Birk Hellenes, Kamil Olejník, Václav Petříček, Petr Doležal, Lukas Horak, Eva Schmoranzerová, Antonín Bad'Ura, Sylvain Bertaina, Andy Thomas, Vincent Baltz, Lisa Michez, Jairo Sinova, Sebastian T. B. Goennenwein, Tomáš Jungwirth, Libor Šmejkal

Nature Communications 15:4961 (2024)10.1038/s41467-024-48493-w

Altermagnetic variants in thin films of Mn5Si3

Javier Rial, Miina Leiviskä, Gregor Skobjin, Antonín Bad'Ura, Gilles Gaudin, Florian Disdier, Richard Schlitz, Ismaïla Kounta, Sebastian Beckert, Dominik Kriegner, Andy Thomas, Eva Schmoranzerová, Libor Šmejkal, Jairo Sinova, Tomáš Jungwirth, Lisa Michez, Helena Reichlová, Sebastian Goennenwein, Olena Gomonay, Vincent Baltz

Physical Review B 110:L220411 (2024)10.1103/PhysRevB.110.L220411

Growth Mechanisms of GaN/GaAs Nanostructures by Droplet Epitaxy Explained by Complementary Experiments and Simulations

Guy Tsamo, Alla Nastovjak, Nataliya Shwartz, Philip Hoggan, Christine Robert-Goumet, Alberto Pimpinelli, Matthieu Petit, Alain Ranguis, Emmanuel Gardés, Mamour Sall, Luc Bideux, Guillaume Monier

Journal of Physical Chemistry C 128:5168-5178 (2024)10.1021/acs.jpcc.3c07945

Covalency versus magnetic axiality in Nd molecular magnets: Nd-photoluminescence, strong ligand-field, and unprecedented nephelauxetic effect in fullerenes NdM2N@C80 (M = Sc, Lu, Y)

Wei Yang, Marco Rosenkranz, Georgios Velkos, Frank Ziegs, Vasilii Dubrovin, Sandra Schiemenz, Lukas Spree, Matheus Felipe de Souza Barbosa, C. Guillemard, Manuel Valvidares, Bernd Büchner, Fupin Liu, Stanislav Avdoshenko, Alexey Popov

Chemical Science 15:2141-2157 (2024)10.1039/d3sc05146c

2023

Competitive actions of MnSi in the epitaxial growth of Mn5Si3 thin films on Si(111)

Ismaïla Kounta, Helena Reichlova, Dominik Kriegner, Rafael Lopes Seeger, Antonin Bad'Ura, Miina Leiviska, Amine Boussadi, Vasile Heresanu, Sylvain Bertaina, Matthieu Petit, Eva Schmoranzerova, Libor Smejkal, Jairo Sinova, Tomas Jungwirth, Vincent Baltz, Sebastian T B Goennenwein, Lisa Michez

Physical Review Materials 7:024416 (2023)10.1103/PhysRevMaterials.7.024416

Large‐Area Synthesis of Ferromagnetic Fe(5−x)GeTe2 /Graphene van der Waals Heterostructures with Curie Temperature above Room Temperature

Hua Lv, Alessandra da Silva, Adriana Figueroa, Charles Guillemard, Iván Fernández Aguirre, Lorenzo Camosi, Lucia Aballe, Manuel Valvidares, Sergio Valenzuela, Jürgen Schubert, Martin Schmidbauer, Jens Herfort, Michael Hanke, Achim Trampert, Roman Engel-Herbert, Manfred Ramsteiner, Joao Marcelo J. Lopes

Small 19 (2023)10.1002/smll.202302387

Engineering of perpendicular magnetic anisotropy in half-metallic magnetic Heusler epitaxial thin films

V. Palin, Charles Guillemard, C. de Melo, Sylvie Migot, P. Gargiani, M. Valvidares, F. Bertran, S. Andrieu

Physical Review Applied 20:054017 (2023)10.1103/PhysRevApplied.20.054017

Paramagnetic Nd sublattice and thickness-dependent ferromagnetism in Nd2NiMnO6 double perovskite thin films

Jonathan Spring, Gabriele de Luca, Simon Jöhr, Javier Herrero-Martín, Charles Guillemard, Cinthia Piamonteze, Carlos Rosário, Hans Hilgenkamp, Marta Gibert

Physical Review Materials 7:104407 (2023)10.1103/PhysRevMaterials.7.104407

Ultrafast demagnetization of Co2MnSi1–xAlx Heusler compounds using terahertz and infrared light

Wei Zhang, Thomas Blank, C. Guillemard, Claudia de Melo, Stéphane Mangin, Alexey Kimel, Stéphane Andrieu, Grégory Malinowski

Physical Review B B 107:224408 (2023)10.1103/physrevb.107.224408

2022

Top‐Layer Engineering Reshapes Charge Transfer at Polar Oxide Interfaces

Gabriele de Luca, Jonathan Spring, Moloud Kaviani, Simon Jöhr, Marco Campanini, Anna Zakharova, Charles Guillemard, Javier Herrero‐martin, Rolf Erni, Cinthia Piamonteze, Marta D Rossell, Ulrich Aschauer, Marta Gibert

Advanced Materials 34:2203071 (2022)10.1002/adma.202203071

Tuning the Mn5Ge3 and Mn11Ge8 thin films phase formation on Ge(111) via growth process

Mohamed-Amine Guerboukha, Matthieu Petit, Aurélie Spiesser, Alain Portavoce, Omar Abbes, Vasile Heresanu, Sylvain Bertaina, Cyril Coudreau, Lisa Michez

Thin Solid Films 761:139523 (2022)10.1016/j.tsf.2022.139523

Control of Oxygen Vacancy Ordering in Brownmillerite Thin Films via Ionic Liquid Gating

Hyeon Han, Arpit Sharma, Holger Meyerheim, Jiho Yoon, Hakan Deniz, Kun-Rok Jeon, Ankit Sharma, Katayoon Mohseni, Charles Guillemard, Manuel Valvidares, Pierluigi Gargiani, Stuart Parkin

ACS Nano 16:6206-6214 (2022)10.1021/acsnano.2c00012

Reversal of Anomalous Hall Effect and Octahedral Tilting in SrRuO3 Thin Films via Hydrogen Spillover

Hyeon Han, Hua Zhou, Charles Guillemard, Manuel Valvidares, Arpit Sharma, Yan Li, Ankit Sharma, Ilya Kostanovskiy, Arthur Ernst, Stuart Parkin

Advanced Materials 35 (2022)10.1002/adma.202207246

Unveiling the atomic position of C in Mn5Ge3Cx thin films

L.-A. Michez, M. Petit, V. Heresanu, V. Le Thanh, E. Prestat, F. d'Acapito, Q. Ramasse, F. Boscherini, P. Pochet, M. Jamet

Physical Review Materials 6:074404 (2022)10.1103/PhysRevMaterials.6.074404

XPS modeling of GaN/GaAs nanostructure grown by the droplet epitaxy technique

Guy Tsamo, Guillaume Monier, Philip Hoggan, Christine Robert-Goumet, Matthieu Petit, Alain Ranguis, Luc Bideux

Journal of Electron Spectroscopy and Related Phenomena 261 (2022)10.1016/j.elspec.2022.147257

2021

Unveiling transport properties of Co2MnSi Heusler epitaxial thin films with ultra-low magnetic damping

C. de Melo, C. Guillemard, A.M. Friedel, V. Palin, J.-C. Rojas-Sánchez, S. Petit-Watelot, Stéphane Andrieu

Applied Materials Today 25:101174 (2021)10.1016/j.apmt.2021.101174

Large-area van der Waals epitaxy and magnetic characterization of Fe3GeTe2 films on graphene

J. Marcelo J. Lopes, Dietmar Czubak, Eugenio Zallo, Adriana, I Figueroa, Charles Guillemard, Manuel Valvidares, Juan Rubio-Zuazo, Jesus Lopez-Sanchez, Sergio O. Valenzuela, Michael Hanke, Manfred Ramsteiner

2D Materials 8:041001-1-041001-8 (2021)10.1088/2053-1583/ac171d

Nanocontact vortex oscillators based on Co$_2$MnGe pseudo spin valves

Jérémy Létang, Claudia de Melo, Charles Guillemard, Aymeric Vecchiola, Damien Rontani, S. Petit-Watelot, Myoung-Woo Yoo, Thibaut Devolder, Karim Bouzehouane, Vincent Cros, Stéphane Andrieu, Joo-Von Kim

Physical Review B 103:224424 (2021)10.1103/PhysRevB.103.224424

2020

Magnetic anisotropy of one-dimensional Co nanostructures

Michel Daher Mansour, Romain Parret, F. Cheynis, Matthieu Petit, Fadi Choueikani, Lisa Michez, Laurence Masson

Physical Review B 102:155403 (2020)10.1103/PhysRevB.102.155403

Issues in growing Heusler compounds in thin films for spintronic applications

C. Guillemard, S. Petit-Watelot, T. Devolder, L. Pasquier, P. Boulet, S. Migot, J. Ghanbaja, F. Bertran, S. Andrieu

Journal of Applied Physics 128:241102 (2020)10.1063/5.0014241

Facilities

UHV equipment for spintronic applications

MBE cluster
(click to enlarge) MBE cluster

Ultrahigh vacuum (UHV) growth system dedicated to Ge/Si-based heterostructures for spintronic applications:

  • A load-lock chamber equipped with a 4 samples holder carousel
  • The main Molecular Beam Epitaxy (MBE) growth chambers:
    • MBE-1: Si, Ge, P, C, Al, Mn
    • MBE-2: metals (Au, Cr, Co, Mn, Ru, Sn etc)
    • OMBE: organic molecules (PTCDI, etc)
  • a preparation chamber (ionic cleaning)
  • A 4 meters long vacuum transfer pipe connecting these three chambers allowing samples transfers without air exposure.

Scheme of the MBE cluster.
(click to enlarge) Scheme of the MBE cluster.

The maximum size of the samples which can be used is 5 cm / 2” in diameter.

The sample holders can be heated up to 1100°C.

We also have:

  • a UHV suitcase to transfer samples
  • an Omicron-type sample plates / molyblock adaptator

 

Effusion and sublimation cells are installed in the MBE chambers:

  • Ge, Mn, Sb, Au
  • Doping cells: Si, C, GaP (P) (SUSI-D, SUKO-D and DECO-D sources respectively, from MBE-Komponenten)

The growth processes and thin films can be characterized in situ by:

  • quartz crystal microbalance
  • RHEED (Reflection high-energy electron diffraction)
  • AES (Auger electrons spectroscopy)

Collaborations

National

  • IM2NP, Marseille
  • CEA, Orsay
  • SPINTEC, Grenoble
  • Institut Néel, Grenoble
  • Institut Pascal, Clermont-Ferrand
  • C2N, Paris

International

  • IFPAN, Varsaw, Poland
  • AIST, Tsukuba (つくば市), Japan
  • University of Stuttgart, Stuttgart, Germany
  • University of Manchester, UK