Terahertz-frequency sensors for atmospheric chemistry and space research

Lead Research Organisation: University of Leeds
Department Name: Electronic and Electrical Engineering

Abstract

When we look into space with existing infrared, radio and microwave sensors, we see less than half the light in our galaxy. Most of this "missing" light lies in the terahertz (THz) or far-infrared part of the spectrum (1-10 THz, 30-300 micron wavelength). Indeed, the "invisible" gases in the Earth's atmosphere and the "dark" dust and gas clouds between stars all glow with distinctive THz fingerprints, providing a wealth of hidden information urgently needed by atmospheric and space scientists.

Despite this great potential, existing THz sensor systems are too large, fragile and complex for most applications outside the laboratory and lack the sensitivity needed for studying reactive gases. Furthermore, this lack of technological readiness limits the prospects for THz systems being deployed in space. A short time-window is available for the UK to invest in real-world demonstrations of key THz components and sensing techniques and secure a place in forthcoming space missions. Without this, the potential for a UK researcher to lead the world in this emerging area will be lost.

In this fellowship, I will overcome the previous limitations of THz gas sensors by developing high-sensitivity systems based on quantum-cascade lasers (QCLs) - QCLs are highly compact sources of THz radiation, which yield >1000 times the power of any similar-sized device.

Unlike previous THz-QCL-based gas-sensing schemes, I will use high-precision analytical chemistry techniques. This will include the use of custom-made reflective cavities and multi-pass gas cells in which THz radiation passes repeatedly through the gas under study, yielding an estimated 100x improvement in sensitivity. I will also work with my project partners in RAL Space to control the frequency of my THz sensors precisely, giving 10x improvement in the resolution of spectral "fingerprints" compared with free-running QCLs. Together these advancements will allow the first laboratory observation of key atmospheric reactions and underpin future deployment in satellite applications.

Specifically, I will develop the first high-precision gas sensors operating in the THz band, with the robustness, compact size and sensitivity needed for installation on a satellite or the International Space Station. The UK and European Space Research communities have taken great interest in THz gas sensing, with at least two in-flight systems currently under consideration. These include "TARDiS" - a UK-led THz astrophysics system for the International Space Station, and "LOCUS" - an Earth-observing THz satellite for studying the climate and space-weather effects in the upper atmosphere.

The same THz instrumentation would allow ultra-precise monitoring of chemical processes in industry or in research laboratories. Trace gases will be revealed, together with the composition of highly-reactive gas species, which cannot be distinguished reliably using existing techniques. Key examples include allowing manufacturers to ensure that vehicles meet strict new emission targets (Euro 6) or allowing atmospheric scientists to understand chemical processes that occur in the upper atmosphere, providing critical missing pieces of information needed to model the Earth's changing climate.

I shall also bring these high-sensitivity techniques into relevant application environments for the first time, through the development of a compact and portable "industrial evaluator" system, containing the complete optical, electronic and cooling systems needed for high-precision THz gas sensing. I will undertake a series of industrial placements with my project partners in the STFC RAL Space division to prove key applications within long-path atmospheric gas sensing. Furthermore, I will build a wider network of academic and industrial beneficiaries to establish and sustain THz gas-sensing as a UK strength within analytical chemistry. Through this, I will initiate the first commercialisation of this new technology.

Planned Impact

This programme is designed to have considerable impact far beyond Academic research and will be sustained beyond the duration of my Fellowship. The beneficiaries of this work include:

1) The UK Space Industry: The UK Industrial Strategy aims to grow this sector to 10% of the £400bn global market by 2030, and Climate applications represent a potential return of >£1bn to UK-based suppliers. This programme will demonstrate key THz components with applications in atmospheric research. This will accelerate their technology readiness level (TRL), enabling their use in space missions such as the LOCUS Upper Atmospheric Satellite, and the TARDiS International Space Station instrument. Specifically, high-precision THz gas sensing will play a key part in international efforts to understand and manage climate change through at least two routes: (i) The first direct mapping of reactive upper-atmospheric species (e.g., O, OH), giving a sensitive indicator of climate change effects. (ii) The first laboratory measurements of short-lived upper-atmospheric species (peroxy radicals and Criegee intermediates) that dictate "greenhouse gas" lifetimes. Earth Observation data and improved climate models will reduce uncertainty in scientific assessment of future emission pathways and climate risk (e.g. through the Intergovernmental Panel on Climate Change Assessment Reports) thereby supporting policy-makers in developing strategies to meet the Paris Agreement targets.

2) Vehicle manufacturers, environmental regulators and testing services: Environmental legislation imposes strict limits on vehicle emissions (e.g., CO). As such, manufacturers and regulators require technology for accurate trace-gas measurements to ensure compliance with targets. The latest European standards (Euro-6) already challenge the spectral-resolution capability of conventional emission-measurement systems. The THz sensors developed in this work will yield environmental impact by providing the sensitivity and resolution needed for such measurements and enable stricter future targets to be monitored. This will impact on the automotive industry by enabling production of commercial portable emissions measurement systems, and their use by testing services.

3) Chemical and process industry: THz sensors will enable precise analysis of gases in industrial process control, e.g., within the petrochemical, biofuels and manufacturing sectors. By monitoring key gas species in emissions, or within reaction vessels, processes can be made cleaner, and more efficient, leading to lower wastage and improved yields, benefiting industry and in turn the UK economy. Urban populations will benefit from the above, through improved air quality and ensuing health benefits.

4) Public health: The development of THz biomedical diagnostics will help improve healthcare. For example, rapid exhaled breath analysis has the potential to replace invasive and slow blood tests or biopsies, with key gas species having been identified as markers for many conditions including asthma, diabetes and gastro-intestinal diseases.

5) Public safety and security: The use of THz trace-gas sensors will enable detection of explosives or chemical agents. Within industrial safety, hazardous gas species (e.g., CO or H2S) will be detectable in factories, mines or confined areas at safe stand-off distances.

Additional economic benefits may be realised through ultra-fast THz transceivers for satellite-to-satellite communications or low-latency links for high-frequency financial trading.
 
Description This programme aims to establish terahertz-frequency (THz) gas sensing as a key technique for atmospheric and space research. The original objectives may be divided broadly into two overarching themes: (1) development of high-precision instruments for THz gas sensing, and (2) demonstration of fast and precise analytical techniques.

In the first regard, I have led the development of THz sources for two proposed UK-led satellite missions - the KEYSTONE (formerly LOCUS) mission to survey key gases in the Earth's upper atmosphere to provide "missing links" in our understanding of climate-change phenomena, and the LETO mission to explore star formation processes in the interstellar medium. The instrumentation development funded through this programme has raised the technical maturity level of both programmes and enabled their highly commended submissions to the European Space Agency for mission funding. I have led the integration of THz quantum-cascade lasers (QCLs) into precision-machined waveguide modules covering the entire 2-5 THz band for the first time. In collaboration with RAL Space, we have developed the first portable and integrated THz receiver demonstrator system, and deployed this in a thermal-vacuum satellite test chamber as part of a series of site visits. I have demonstrated also the first integration of a THz QCL with a ring-resonator device to provide compact and high-speed stabilisation of the laser power and independent control of the emission frequency. I have also demonstrated the first liquid-crystal based modulators for use at >1 THz, allowing long-term correction against power drifts in future satellite instruments.

I have pioneered a range of high-precision THz sensing techniques and associated instrumentation. By exploiting the self-mixing effect (i.e., intentionally inducing feedback within QCLs), I have shown that rapid and "detector free" measurements of gas concentrations can be obtained. I have shown also that acoustic waves can be used to control the dynamics of THz QCLs, potentially enabling their use in ultrafast gas analysis techniques. In collaboration with the laser spectroscopy group at RAL Space, I have developed the design of a multi-pass THz gas spectroscopy system, potentially enabling two orders of magnitude improvement in gas detection sensitivity compared with conventional approaches. I have also developed a new collaboration with Goethe University Frankfurt to demonstrate gas sensing at the sub-microsecond timescales needed for future UV-pump photolysis measurements of reactive gas species.
Exploitation Route The compact and integrated THz instrumentation developed in this work will underpin future satellite systems for Earth observation and deep-space astronomy on the 5-10 year timescale. The "downstream" data from these missions will enable atmospheric and climate researchers to fill in missing links in climate models (e.g., greenhouse gas lifetimes in the presence of volatile-organic compounds), and in star-formation processes in deep-space nebulae.

Beyond this, the high-speed and stabilised THz instrumentation developed in this programme will underpin potential applications in ultrafast wireless communications, security imaging and biomedical sensing (e.g., skin-cancer imaging).

The analytical chemistry techniques being developed in this programme will underpin laboratory-based analysis of atmospheric reactions under controlled conditions. This will also be of potential benefit for industrial process control, vehicle emissions sensing, and agricultural monitoring applications.
Sectors Aerospace, Defence and Marine,Agriculture, Food and Drink,Digital/Communication/Information Technologies (including Software),Electronics,Security and Diplomacy

 
Description The findings of this work (principally, the development of the first compact, and integrated THz systems) has underpinned the design and development of two new satellite mission concepts, as part of two international teams. The KEYSTONE atmospheric sounding mission has been submitted as a candidate for the European Space Agency (ESA) Earth Explorer programme, and aims to provide the first global mapping of key gas species in the Earth's upper atmosphere, using THz receivers, and providing critical missing data for climate models. The "LETO" satellite concept has also been submitted as an ESA medium-scale mission to the L2 Lagrangian point, providing whole-sky THz spectroscopic mapping, and yielding the first detailed analysis of star formation processes in the interstellar medium. As an invited academic presenter, Dr Valavanis has engaged in round-table consultations with senior leaders from UK industry as part of the CEOI Industrial Consultation Workshop on Millimetre-Wave, Microwave and Terahertz Remote Sounding. The discussion incorporated the results of this programme, including the newly developed compact THz spectroscopy apparatus and integration techniques. This meeting led to the publication of a consultation document, which has been circulated to the CEOI's full industrial beneficiary network. It will be used by the CEOI and the wider UK Space Agency to inform the focus for future funding and to maximise the potential for space-related technologies to be used in wider non-space industrial fields. Dr Valavanis has also contributed to the development of Space Hub Yorkshire (SHY), and has contributed to SHY round-table discussions, linking academic, industrial and public sector bodies.
First Year Of Impact 2020
Sector Aerospace, Defence and Marine,Chemicals,Environment,Healthcare,Pharmaceuticals and Medical Biotechnology
Impact Types Societal,Economic,Policy & public services

 
Description 2.0 THz local oscillators for radiometric observation of atomic oxygen
Amount £225,962 (GBP)
Funding ID RP10G0435A504 
Organisation UK Space Agency 
Sector Public
Country United Kingdom
Start 04/2022 
End 02/2023
 
Description Acoustic control of quantum cascade heterostructures: the THz "S-LASER"
Amount £998,933 (GBP)
Funding ID EP/V004743/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 12/2021 
End 11/2024
 
Description Advanced manufacturing techniques for supra-terahertz optical components
Amount £73,839 (GBP)
Funding ID NSTP3-PF3-078 
Organisation UK Space Agency 
Sector Public
Country United Kingdom
Start 11/2020 
End 03/2021
 
Description Design, Fabrication and Testing of Calibration Targets for the Calibration of Supra-THz Channels, up to 4.7 THz
Amount € 300,000 (EUR)
Funding ID 4000138393/22/NL/AS 
Organisation European Space Agency 
Sector Public
Country France
Start 07/2022 
End 12/2023
 
Description Terahertz frequency devices and systems for ultrahigh capacity wireless communications
Amount £7,097,283 (GBP)
Funding ID EP/W028921/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 01/2023 
End 12/2027
 
Title Dataset associated with "All-electronic phase-resolved THz microscopy using the self-mixing effect in a semiconductor laser" 
Description This dataset relates to data presented in the work, "All-electronic phase-resolved THz microscopy using the self-mixing effect in a semiconductor laser". In this work we report all-electronic coherent scattering-type scanning near-field microscopy (s-SNOM) using a terahertz-frequency quantum cascade laser. By exploiting the coherent self-mixing effect in these lasers, in conjunction with electronic frequency tuning of the laser, we demonstrate spatial mapping of both the amplitude and phase of the scattered field with deeply sub-wavelength resolution. We apply our technique for coherent microscopy of a phonon-resonant crystal. The extracted amplitude and phase parameters reveal clear contrast when compared to both metallic and non-resonant dielectric materials, and show excellent agreement with those calculated using a finite-dipole model of the near-field interaction between the s-SNOM tip and the resonant sample in the Reststrahlen band. 
Type Of Material Database/Collection of data 
Year Produced 2021 
Provided To Others? Yes  
Impact This data underpinned publication of an ACS Photonics article, and demonstrated the highest-resolution phase-resolved THz microscopy to date. This will, in turn, enable plasmonic or chemical sensing on the few-nanometre scale. 
URL http://archive.researchdata.leeds.ac.uk/835/
 
Title Dataset associated with 'High-Speed Modulation of a Terahertz Quantum Cascade Laser by Coherent Acoustic Phonon Pulses' 
Description This archive contains the dataset associated with the publication entitled 'High-Speed Modulation of a Terahertz Quantum Cascade Laser by Coherent Acoustic Phonon Pulses'. Fast modulation of lasers is a fundamental requirement for applications in optical communications, high-resolution spectroscopy and metrology. In the terahertz-frequency range, the quantum-cascade laser (QCL) is a high-power source with the potential for high-frequency modulation. However, conventional electronic modulation is limited fundamentally by parasitic device impedance, and so alternative physical processes must be exploited to modulate the QCL gain on ultrafast timescales. Here, we demonstrate an alternative mechanism to modulate the emission from a QCL device, whereby optically-generated acoustic phonon pulses are used to perturb the QCL bandstructure, enabling fast amplitude modulation that can be controlled using the QCL drive current or strain pulse amplitude, to a maximum modulation depth of 6% in our experiment. We show that this modulation can be explained using perturbation theory analysis. While the modulation rise-time was limited to ~800 ps by our measurement system, theoretical considerations suggest considerably faster modulation could be possible. Data included: power-current (L-I), power-voltage (L-V) data; Voltage across QCL device and Schottky signal detected from device for different bias conditions; Magnitudes of acoustic modulation shown in Figure 4; Resonant tunnelling data from Figure 5; Simulation .mat file for predicted power modulation shown in figure 3 (b). 
Type Of Material Database/Collection of data 
Year Produced 2020 
Provided To Others? Yes  
Impact This dataset underpinned a Nature Communications paper (DOI:10.1038/s41467-020-14662-w), in which the first ultra-fast modulation of a THz quantum-cascade laser using bulk acoustic waves was reported. This has the potential for use in high-speed communications, coherent sensing or mode-locking applications. 
URL http://archive.researchdata.leeds.ac.uk/634/
 
Description Max-IR Labs 
Organisation Max IV Laboratory
Country Sweden 
Sector Academic/University 
PI Contribution Fabrication and custom-mounting of terahertz-frequency quantum-cascade lasers, for use in infrared thermometry experiments
Collaborator Contribution Provision of customised mounting components for terahertz quantum-cascade lasers, and provision of staff/facility time for experimental analysis of the thermal properties of THz QCLs using novel infrared-fibre-optic themometry systems.
Impact This collaboration provided mutual benefit to The University of Leeds, and Max-IR Labs, through the first attempt to measure the microscopic thermal properties of a THz QCL using an infrared-fibre-based thermometric sensor. Although the system was unable to detect thermal emissivity, this collaboration provided an important initial assessment of system sensitivity, and will inform future design of the thermal microscopy technique. Ultimately, this will underpin economic impact through improving the system integration design (i.e., thermal management) for high-powered THz devices, which in turn is a key enabling step to the delivery of satellite and industrial systems for atmospheric and space research (e.g., the analysis of chemical pathways underpinning climate change phenomena). In turn, these measurements provide an important test-bed for the Max-IR Labs commercial thermometry system, which will be an enabling technology for developing efficient heat management in semiconductor microelectronics.
Start Year 2019
 
Description Rutherford Appleton Labs - FLF partnership 
Organisation Rutherford Appleton Laboratory
Department RAL Space
Country United Kingdom 
Sector Academic/University 
PI Contribution Fabrication and optimisation of terahertz-frequency quantum-cascade lasers for use in integrated satellite-borne receivers. Characterisation of integrated QCL devices and far-field THz power mapping. Development and calibration of multi-pass gas spectroscopy instrumentation.
Collaborator Contribution Development of micromachined waveguides and antennas for THz sources; integration of THz sources with Schottky-barrier mixers; characterisation of materials; phase-locking of THz sources; provision of bespoke gas-cell optics; simulation and analysis of THz gas spectra.
Impact Invited conference presentations at CLEO, San Jose (DOI:10.1364/CLEO_AT.2019.AW3P.5) and IEEE MTT-S, Guangzhou (DOI:10.1109/IEEE-IWS.2019.8803875). This is a multi-disciplinary collaboration, bringing together expertise in laser spectroscopy (D. Weidmann, RAL Space), atmospheric retrieval simulations (D. Gerber, RAL Space), millimetre-wave engineering and manufacturing (B. Ellison & D. Pardo, RAL Space), with atmospheric chemistry (J. Lehman, Leeds) and THz quantum-cascade instrumentation (A. Valavanis, Leeds)
Start Year 2019
 
Description TeraFET development 
Organisation Goethe University Frankfurt
Country Germany 
Sector Academic/University 
PI Contribution Characterisation of TeraFET detectors, and applications development. Hosting of two visiting postgraduate researchers during placement visits. Laboratory access, and design consultation from senior academic staff. Contribution to the writing of a successful DFG funding proposal to develop THz mixers and fast detectors based on FET technology.
Collaborator Contribution Design and supply of TeraFET detectors at frequencies applicable to quantum-cascade laser sources. Meetings and design consultations with senior academic staff.
Impact Successful DFG funding proposal to develop THz mixers and fast detectors based on FET technology.
Start Year 2022
 
Description BeCurious Festival 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Public/other audiences
Results and Impact I delivered an introductory talk to the general public on THz atmospheric and Space Research as part of the BeCurious research festival. This was followed by questions from the audience and discussions about THz technology.
Year(s) Of Engagement Activity 2021
URL https://youtu.be/UiGgxdEoHdk
 
Description CEOI Industrial Consultation Workshop on Millimetre Wave, Microwave and THz Remote Sensing 
Form Of Engagement Activity A formal working group, expert panel or dialogue
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Industry/Business
Results and Impact Following grant support for a number of projects to companies developing millimetre wave, microwave and THz remote sensing technologies (30MHz to 3THz), CEOI ran the Workshop to inform senior industrial technical directors and managers, and to further explore potential uses in wider industrial applications.

The consultation brought together industry representatives and leading academics in this emerging field. Attendees were from aerospace, communications, defence, environmental, healthcare, instrumentation, and oil & gas organisations. It provided a fascinating opportunity for participants to contribute ideas, identify future needs, learn, discuss, and network.

The outputs will inform the focus of future CEOI and UKSA funding programmes. Specifically targeting remote sensing applications, the meeting aimed to:

• Understand potential market developments and applications in millimetre wave, microwave and THz remote sensing and their market drivers;
• Identify key barriers and technical challenges to their implementation;
• Investigate the possibility of brokering relationships with interested parties along the supply chains for promising new applications / markets;
• Create opportunities for attendees to network across the different communities.
Year(s) Of Engagement Activity 2019
URL https://ceoi.ac.uk/events/previous-events/industry-consultation-workshops/
 
Description CEOI Industry Consultation Workshop - Miniaturisation of Millimetre, Microwave & Terahertz Remote Sensing 
Form Of Engagement Activity A formal working group, expert panel or dialogue
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Industry/Business
Results and Impact Following grant support for a number of projects to companies and universities for
miniaturisation of millimetre, microwave and terahertz remote sensing technologies, CEOI ran a
Workshop to inform senior industrial technical directors and managers of the new technology
developments, and to further explore potential uses in wider industrial applications.
The consultation brought together industry representatives and leading academics in the field.
Attendees were from the consulting, defence, environment, oil & gas, telecoms, and new space
sectors. It provided a unique opportunity for participants to hear of the latest research outcomes
in the domain, contribute ideas, identify future needs, discuss, and network.
The outputs will inform the focus of future CEOI and UKSA strategies and programmes.
Specifically targeting remote sensing applications, the meeting aimed to:
• Inform attendees of some of the latest technical developments in miniaturisation of
millimetre, microwave and terahertz remote sensing
• Understand potential market developments / applications in the domain and the research
focus for the next generation
• brainstorm with industry representatives the key opportunities and technical challenges in
their further development and wider deployment
• investigate the possibility of brokering relationships with interested parties along the
supply chains for promising new applications / markets
• create opportunities for attendees to network across the different communities
Year(s) Of Engagement Activity 2022
 
Description Cafe Scientifique - Headingley 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach Local
Primary Audience Public/other audiences
Results and Impact I delivered a public outreach talk to a general public audience of approximately 50 people. There was a lively question and answer session afterwards, with many audience members noting this as the first time they had been aware of terahertz science and technology.
Year(s) Of Engagement Activity 2022
URL http://cafesci.hdtleeds.org.uk/wp-content/uploads/2022/10/TerahertzWaves-AlexValavanis20221010.pdf
 
Description Lancaster University Research Seminar 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Postgraduate students
Results and Impact I was the invited speaker for a research seminar at Lancaster University in January 2020. A presentation on the FLF research programme was delivered to approx. 50 academic staff, postgraduate and undergraduate students. This was followed by an extended questions and answers session with the audience, and detailed discussions with Lancaster University staff about potential future collaborative activities in THz modulator systems.
Year(s) Of Engagement Activity 2020
 
Description Quantum Sauce - "Good Vibrations 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach Local
Primary Audience Public/other audiences
Results and Impact I delivered a public outreach talk to a general public audience of approximately 50 people. There was a lively question and answer session afterwards, with many audience members noting this as the first time they had been aware of terahertz science and technology.
Year(s) Of Engagement Activity 2022
URL https://www.eventbrite.co.uk/e/quantum-sauce-good-vibrations-tickets-333629032417
 
Description Tsinghua University Physics Forum 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Postgraduate students
Results and Impact I was the invited speaker for the Tsinghua University Physics Forum in October 2019. A presentation on the FLF research programme was delivered to approx. 50 academic staff, postgraduate and undergraduate students. This was followed by an extended questions and answers session with the audience, and estabished a link with Tsinghua University staff to explore potential transnational activities in THz adaptive optics research.
Year(s) Of Engagement Activity 2019