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.

Group leader

Researchers

University Lecturer

Postdoctoral fellow

PhD Student

Publications

2024

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

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

2022

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

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

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

Selective modification of the unquenched orbital moment of manganese introduced by carbon dopant in epitaxial Mn5Ge3C0.2/Ge(111) films

R. Kalvig, E. Jedryka, M. Wojcik, Matthieu Petit, L. Michez

Physical Review B: Condensed Matter (1978-1997) 101 (2020)10.1103/PhysRevB.101.094401

Electrolyte-gated-organic field effect transistors functionalized by lipid monolayers with tunable pH sensitivity for sensor applications

Tin Phan Nguy, Ryoma Hayakawa, Volkan Kilinc, Matthieu Petit, Yemineni S L V Narayana, Masayoshi Higuchi, Jean-Manuel Raimundo, Anne Charrier, Yutaka Wakayama

Applied Physics Express 13:011005 (2020)10.7567/1882-0786/ab5322

2019

Stable operation of water-gated organic field-effect transistor depending on channel flatness, electrode metals and surface treatment

Tin Phan Nguy, Ryoma Hayakawa, Volkan Kilinc, Matthieu Petit, Jean-Manuel Raimundo, Anne Charrier, Yutaka Wakayama

Japanese Journal of Applied Physics 58:SDDH02 (2019)10.7567/1347-4065/ab09d2

Step flow growth of Mn5Ge3 films on Ge(111) at room temperature

Matthieu Petit, Amine Boussadi, Vasile Heresanu, Alain Ranguis, Lisa Michez

Applied Surface Science 480:529-536 (2019)10.1016/j.apsusc.2019.01.164

2018

Hyperfine fields and anisotropy of the orbital moment in epitaxial Mn5Ge3 films studied by Mn55 NMR

R. Kalvig, E. Jedryka, M. Wojcik, G. Allodi, R. de Renzi, Matthieu Petit, Lisa Michez

Physical Review B: Condensed Matter and Materials Physics (1998-2015) 97:174428-174428 (2018)10.1103/PhysRevB.97.174428

From the very first stages of Mn deposition on Ge(001) to phase segregation

Sion F Olive Mendez, Matthieu Petit, Alain Ranguis, Vinh Le Thanh, Lisa Michez

Crystal Growth & Design 18:5124-5129 (2018)10.1021/acs.cgd.8b00558

Investigations of the Anodic Porous Etching of n-InP in HCl by Atomic Absorption and X-ray Photoelectron Spectroscopies

Lionel Santinacci, Muriel Bouttemy, Matthieu Petit, Anne-Marie Goncalves, Nathalie Simon, Jackie Vigneron, Arnaud Etcheberry

Journal of The Electrochemical Society 165:3131-3137 (2018)10.1149/2.0181804jes

Thiol-functionalization of Mn5Ge3 thin films

Marta K Schütz, Matthieu Petit, Lisa Michez, Alain Ranguis, Guillaume Monier, Christine Robert-Goumet, Jean-Manuel Raimundo

Applied Surface Science 451:191-197 (2018)10.1016/j.apsusc.2018.04.231

2017

Study of manganese germanides formation and their magnetic response

Omar Abbes, Alain Portavoce, Christophe Girardeaux, Lisa Michez, Vinh Le Thanh

Advanced Materials Letters 8:600-604 (2017)

Atomic layer deposition of HfO2 for integration into three-dimensional metal–insulator–metal devices

Loïc Assaud, Kristina Pitzschel, Maïssa K. S. Barr, Matthieu Petit, Guillaume Monier, Margrit Hanbücken, Lionel Santinacci

Applied physics. A, Materials science & processing 123:768 (2017)10.1007/s00339-017-1379-2

Ferromagnetic resonance in Mn 5 Ge 3 epitaxial films with weak stripe domain structure

R Kalvig, E Jedryka, P. Aleshkevych, M Wojcik, W Bednarski, Matthieu Petit, L. Michez

Journal of Physics D: Applied Physics 50:125001 (2017)10.1088/1361-6463/aa5ce5

2016

Synthesis and Study of Stable and Size-Controlled ZnO-SiO2 Quantum Dots: Application as a Humidity Sensor

Mohamed Aymen Mahjoub, Guillaume Monier, Christine Robert-Goumet, François Reveret, Mosaab Echabaane, Damien Chaudanson, Matthieu Petit, Luc Bideux, Bernard Gruzza

Journal of Physical Chemistry C 120:11652-11662 (2016)10.1021/acs.jpcc.6b00135

An introduction to photocatalysis through methylene blue photodegradation

Matthieu Petit, Lisa Michez, Jean-Manuel Raimundo, Tuhiti Malinowski, Philippe Dumas

European Journal of Physics 37:065808 (2016)10.1088/0143-0807/37/6/065808

Electrical and optical measurements of the bandgap energy of a light-emitting diode

Matthieu Petit, Lisa Michez, Jean-Manuel Raimundo, Philippe Dumas

Physics Education 51:025003 (2016)10.1088/0031-9120/51/2/025003

Mn5Ge3C0.6/Ge(111) Schottky contacts tuned by a n-type ultra-shallow doping layer

Matthieu Petit, Ryoma Hayakawa, Yutaka Wakayama, Vinh Le Thanh, Lisa Michez

Journal of Physics D: Applied Physics 49:355101 (2016)10.1088/0022-3727/49/35/355101

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