Investigating pressure induced conductive states on the nanoscale : A novel route to nano-circuitry

Lead Research Organisation: Queen's University Belfast
Department Name: Sch of Mathematics and Physics

Abstract

The ability to transfer nanometer scale metallic patterns at low cost, high throughput and high resolution has huge implications for slashing the manufacturing costs of semiconductors and data storage devices. Techniques like nanoimprint lithography allow fabrication of such nanometer scale patterns by mechanical deformation of imprint resist and subsequent processes. Even though the technique is considered one of the simplest lithography approaches, it still comprises of several complicated steps during pattern transfer. If the transfer step could be eliminated and only the imprint step could directly result in the printing of a few nanometer sharp circuit pattern on the chosen material, that would represent a dramatic leap in terms of throughput and reproducibility of patterns for nano-circuitry. In order to achieve this visionary goal of directly imprinting circuitry, it is necessary as a first step to understand the physical phenomena in materials that would allow localised pressure to be used as a tool to sketch and control sharp conductive channels in an otherwise insulating material. There are atleast two different mechanisms that could give rise to local pressure induced conductive states in an insulating material. Ferroelectrics with conducting domain walls and materials undergoing metal-insulator phase transitions are the two primary material systems where nanoscale pressure can be used to realise confined conducting states in the material and potentially achieve deterministic control of such interfaces. Both systems allow co-existence of conducting walls or phases in the bulk but the mechanisms through which localised stress results in the formation of conductive interfaces or channels in these materials remains to be well understood before the effect itself can be fully exploited. For potential applications, it is also necessary to evaluate the ease of channel formation under pressure, their stability and reconfigurability. To address these issues, the primary goal of this proposal is to establish the pressure mediated control of localised nanoscale conductive states and develop a fundamental understanding of the physics associated with this behaviour so that reliable control of conductive interfaces can be achieved as a first step towards nano-circuitry. Pressure applied via an atomic force microscope (AFM) tip will be used to inject conductive states in three different materials : an improper ferroelectric, a mixed phase ferroelectric and a material undergoing metal-insulator phase transition, each representing a unique type of conductive interface created through pressure induced writing. In each of the three cases, the achievable degree of control of tip pressure induced conductive walls/phases will be evaluated and experiments will be performed to identify the physical origin and the mechanisms underlying the conductivity of the created interfaces. With a grasp on the mechanism of pressure induced conductivity in these materials, we aim to be able to precisely control the formation and annihilation of these confined walls or phases. The complementarity of pressure mediated control of conductive behaviour with other stimuli will be evaluated for optimal reconfigurability of conductive channels and read/erase capability. Proof-of-concept demonstration of pressure induced conductive channels between lateral electrodes will be performed. The AFM based approach developed here would thus help establish the underpinning physics of pressure induced conductive states in the discussed material systems and provide key insight for developing other nanoimprint methods for direct writing of nano-circuitry.

Planned Impact

The proposal, with its theme focussed around the investigation of pressure induced conducting states in ferroelectrics and materials undergoing phase transitions, has great potential towards delivering significant impact in terms of novel physics as well as development of new technologies based upon the phenomena. The investigated phenomena represents an exciting but relatively unexplored direction and the physics underpinning localised pressure induced conductivity mediated by interfaces like domain walls or metallic phases in materials is novel. The physical understanding of the evolution of ferroelectric domain structures and their control with local mechanical pressure could provide an alternative and complementary route to controlling wall motion, ideas that are likely to create a widespread impact in the domain wall functionality research community as well as researchers working in the area of domain wall nanoelectronics. With these topics emerging as 'hot' areas of research across the world, this proposal will give UK research the potential for making ground-breaking progress. The proposal will also help foster strong international collaborations with teams engaged in research on relevant topics. The proposal will also enable training the next generation of scientists in the evolving and competitive field of nanoscale functional materials. It is foreseen that results and understanding gleaned from the project would generate future projects which are likely to permeate towards undergraduate teaching, especially in the form of MSci projects.

Impact of this proposal to the society will be through successive implementation of our proof-of-concept results towards advanced applications. The broader vision of the proposal, of which the proposed experiments are only a first step, is to develop nanoimprint methods which allow direct writing of nanometers sharp circuitry. This vision, when realised to its full potential, could enable transfer of nanometer scale metal-like patterns at low cost, high throughput and high resolution and has huge implications for slashing the manufacturing costs of semiconductors and data storage devices. The methodology and understanding of the phenomena developed in the proposal could thus enable cheaper and better processing techniques which in turn could bring down the cost of electronic devices and make them more accessible to society increasing the quality of life in UK. As discussed earlier, the ability to utilise localised pressure to control domain walls also opens up possibilities towards the field of domain wall nanoelectronics, a research area which is likely to attract interest from industry. The domain walls can be injected or annihilated by external fields which gives way to their potential use in "active" two dimensional electronic devices and localised stress confined to nanoscale volumes can be used to control their functionality. The potential for control of metal-insulator transition in oxides via localised pressure has significant implications towards novel sensor applications.

Publications

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Campbell M (2016) Hall effect in charged conducting ferroelectric domain walls in Nature Communications

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Kumar A (2020) Nanodomain patterns in ultra-tetragonal lead titanate (PbTiO3) in Applied Physics Letters

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Pradhan DK (2019) Studies of Multiferroic Palladium Perovskites. in Scientific reports

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Schilling A (2016) Reconsidering the origins of Forsbergh birefringence patterns in Physical Review B

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Tikhonov Y (2022) Polarization Topology at the Nominally Charged Domain Walls in Uniaxial Ferroelectrics. in Advanced materials (Deerfield Beach, Fla.)

 
Description One of the key findings achieved from the award has been published in the High-impact journal Nature Communications (https://www.nature.com/articles/ncomms15105) with the employed PDRA as the lead author on the paper. The finding arising from the undertaken research shows that site-specific injection of conducting walls (interfaces) of up to hundreds of microns in length can be achieved through locally applied point-stress in a studied material system and,once created, that they can be moved and repositioned using applied electric fields. The results has implications towards creating and moving conducting walls to make or break electrical connections in new forms of reconfigurable nanocircuitry and adaptive nanoelectronics. This finding has attracted considerable media attention as indicated by the coverage from news sources, scientific blogs and media outlets (https://www.nature.com/articles/ncomms15105/metrics). More recently, the same methodology has been used to discover counter-intuitive domain wall motion in Boracites which implies negative capacitance and can be harnessed for energy efficient next-generation transistors.
Exploitation Route We believe that the findings present a new paradigm to reconfigurable nanocircuitry since creating such long nanometer sharp rectilinear conducting interfaces had not been possible using the existing approaches. Moreover, the approach demonstrated here is a relatively simple one (application of localised stress in improper ferroelectrics) that could be easily adopted by the domain wall nanoelectronics research community. From a technological perspective, the results can be applied towards design of a 'nano-stamp' that could allow single step direct imprinting of conducting channels on to the chosen material and completely eliminate the transfer steps resulting in slashing of manufacturing costs for nano-patterning applications. The expansion of these ideas have now enabled a thriving collaboration between QUB and UCD where we are joining efforts to investigated nano-machining via stress applied via an AFM tip in the plastic regime. Other expansive ideas such as Mechanochemistry etc. are being investigated as part of the ongoing effort.
Sectors Electronics,Manufacturing, including Industrial Biotechology

URL https://www.nature.com/articles/ncomms15105/metrics
 
Description The project aimed to investigate novel ways of employing nanoscale stress to inject conducting domain states in materials with the objective of using them towards nanoscale circuitry. We have focussed on using novel and only recently developed high stiffness tips (with collaboration from Adama Tips and UCD) to undertake the same. In the process of using these tips which are about 100-1000 times stiffer than regular tips for the primary objectives of this proposal, we have found that the same tips can also be used to create nanoindentation on any surface and the same has caught interest from Seagate, one of the largest makers of Hard drives, who are keen to employ such techniques in evaluating site-specific hardness values on the nanometer scale. The approach of AFM tip-assisted milling of precise metallic electrodes and plasmonic nanostructures has now been developed and a CDT-Seagate-funded student is employing it to assess suitability to heat assisted magnetic recording mediated by plasmonic heating. Another CDT project has explored the employability and robustness of the tip-mediated stressing towards fully quantitative hardness measurements on wafers. 3 PhD students (2 indirectly benefitted and 1 directly allocated towards the project) have graduated and entered the local Belfast industry in different types of roles. The PDRA associated with the project has now secured a permanent lectureship at QUB and the grant provided a well-timed mechanism to keep the candidate in academia. As an outcome of this grant, we have also formed strong working collaborations with Adama Technologies (a diamond tip manufacturer) who have provided us letter of support for an EPSRC-SFI grant where they will engage directly with us in terms of tip-design towards the vision of stress-mediated nanocircuitry enabled by control of ferroelectric domain microstructures. Oxford instruments (discussions opened via this grant and enhanced through purchase of a state-of-the-art atomic force microscope in 2018 ) have been a consistent partner supporting our research but also are seeking opportunities towards future patents working with us. In the Grant submitted in 2022, these industrial partners are providing key support for the proposal to facilitate the objectives of the proposal. A tangential impact of the project has been the realisation (initially unintended) that very precise nanomachining better than Focussed ion beam milling can be achieved via tip-enabled stress. This allows micro/nano-fabrication of ferroelectric capacitor structures and also very precise shaping of electrodes and plasmonic nanostructures. The uptake of this method by other CDT students and members of the broader ferroelectric community is creating a lot of excitement and is leading to the realisation that AFM could provide a very effective way of creating well milled defect-free nanostructures.
First Year Of Impact 2020
Sector Electronics,Manufacturing, including Industrial Biotechology
Impact Types Societal,Economic

 
Description Antiferroelectricity, Ferrielectricity and Ferroelectricity in the Archetypal Antiferroelectric PbZrO3 at small scale
Amount £1,200,000 (GBP)
Funding ID USI-211 
Organisation Department for the Economy, Northern Ireland 
Sector Public
Country United Kingdom
Start 08/2022 
End 07/2026
 
Description DTP 2016-2017 Queen's University of Belfast
Amount £2,553,399 (GBP)
Funding ID EP/N509541/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 09/2016 
End 09/2021
 
Description Quantitative Hall Voltage mapping at conducting Ferroelectric domain walls: A novel approach to extracting conduction mechanisms on the nanoscale
Amount £49,693 (GBP)
Funding ID EP/S037179/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 07/2019 
End 06/2020
 
Title Precise nanostructuring of metal electrodes using AFM mediated stress 
Description In this work, we systematically investigate the effect of AFM parameters on the machining behavior of an epitaxially-strained thin film of BiFeO3, a lead-free ferroelectric where the epitaxial constraint gives rise to coexistence of different phases. Such films are prime candidates for magnetoelectric, piezoelectric, and nanoelectronic devices. Here, the conditions required to thin local regions of such a mixed phase BiFeO3 film to a range of depths are theoretically predicted and experimentally demonstrated. These conditions could be utilized for the fabrication of complex 3D nanostructures, measurements of certain properties as a function of thickness, or in some cases alterations of ferroelectric properties due to local changes in the film thickness. A framework is established to determine the optimum conditions required to fabricate nanostructures with the smallest lateral dimensions possible in the film. Finally, the possibility of fabricating a range of different nanostructures is explored. 
Type Of Material Improvements to research infrastructure 
Year Produced 2020 
Provided To Others? Yes  
Impact Atomic force microscopy (AFM) has been utilized for nanomechanical machining of various materials including polymers, metals, and semiconductors. Despite being important candidate materials for a wide range of applications including data storage and actuators, ferroelectric materials have rarely been machined via AFM. AFM-based machining of ferroelectric nanostructures offers advantages over established techniques, such as bottom-up approaches and focused ion beam milling, in select cases where low damage and low-cost modification of already-fabricated thin films are required. Through a systematic investigation of a broad range of AFM parameters, we demonstrate that AFM-based machining provides a low-cost option to rapidly modify local regions of the film, as well as fabricate a range of different nanostructures, including a nanocapacitor array with individually addressable ferroelectric elements. 
URL https://aip.scitation.org/doi/full/10.1063/1.5133018
 
Description Collaboration with Prof. Laurent Bellaiche 
Organisation University of Alabama at Birmingham
Department Department of Physics
Country United States 
Sector Academic/University 
PI Contribution The QUB team has undertaken the experimental investigations of reversible control of mixed phase conductive states in epitaxially strained bismuth ferrite thin films and shown that the goal can be achieved employing nanoscale electrical bias and mechanical stress under a scanning probe tip.
Collaborator Contribution University of Alabama team have undertaken first principle free energy based calculations to provide a theoretical basis for the stress induced phase reorganisation (which creates conductive interfaces) in bismuth Ferrite. Observed field-induced microstructures were found to be consistent with first-principles-based effective Hamiltonian simulations: calculated energy curves predict equilibrium R-T phase populations for different epitaxial strains, applied uniaxial stresses and electric fields, which map well to the observed metastable microstructures imaged after such fields have been applied and then removed.The combination of theory and experiment has laid down the basis for introducing and removing Rhombohedral-tetragonal interfaces and show that the resistance state in the BiFeO3 can be reversibly switched with a maximum "ON-OFF" ratio in resistance of up to six orders of magnitude.
Impact 'Deterministic Reversible Control over Symmetry States in Mixed Phase BiFO3 using Electrical Bias and Uniaxial Stress towards Piezoresistive Applications' IN SUBMISSION, D. Edwards, N. Browne, K. Holsgrove, A. Naden, S. O. Sayedaghaee, B. Xu, S. Prosandeev, D. Wang, D. Mazumdar, A. Gupta, S.V. Kalinin, M.A. Arredondo, R. G. P. McQuaid, L. Bellaiche, J. M. Gregg and A. Kumar
Start Year 2016
 
Description Headstart Physics Summer School 
Form Of Engagement Activity Participation in an open day or visit at my research institution
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Schools
Results and Impact About 50 GB A-Level students attended a residential Head start physics school where I presented a talk relevant to my research activity and presented demonstrations of a LEGO-AFM (custom designed and built by me using this research grant). The demonstration generated several questions and interest among the students some of whom are currently considering joining QUB for their undergraduate physics degree.
Year(s) Of Engagement Activity 2018
 
Description SPM Workshop 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach Regional
Primary Audience Postgraduate students
Results and Impact About 50 PG students and other researchers from Ulster University attended the workshop and asked questions about the use of atomic force microscopy in their research. Discussions with Research PIs have lead to research clollaborations and a new AFM funded by EPSRC is being purchased at UU.
Year(s) Of Engagement Activity 2019