HyperTerahertz - High precision terahertz spectroscopy and microscopy

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

Abstract

The last 20 years have witnessed a remarkable growth in the field of THz frequency science and engineering, which has matured into a vibrant international research area. The modern THz field arguably began with the development of a pulsed (single-cycle) THz emitter - the semiconductor photoconductive switch - and the subsequent development of THz time-domain spectroscopy (TDS). Since then, considerable success has been achieved in the further development of this and other THz sources, including the uni-travelling carrier (UTC) photodiode and the quantum cascade laser (QCL). However, notwithstanding this, it is only the THz-TDS technology that has been developed sufficiently for commercialization as a complete system, leaving other THz devices, components and techniques still restricted to the academic laboratory. This is unfortunate, since despite the success of THz-TDS, the technique has a number of shortcomings including its high fs-laser dominated cost, low power, and limited frequency and spatial resolution, which could be addressed by QCL and UTC technologies if they were to be engineered into appropriate instruments.

In fact, a cursory comparison with the neighbouring microwave and optical regions of the spectrum reveals that THz frequency science and technology is still in its infancy, and not just in the context of commercial uptake. For example, the THz region significantly lags in the availability of precision spectroscopy instrumentation required to address sharp spectral features inherent to gases, for example, in atmospheric analysis, or in materials with long excited state lifetimes. THz technology also significantly lags in the fields of non-linear spectroscopy and coherent control, where powerful and controlled pulses of electromagnetic radiation interact with matter and manipulate its properties. In the optical and microwave regions, fascinating phenomena including electron-spin resonance and nuclear magnetic resonance were major breakthroughs, revealing a wealth of new science and engineering applications. These techniques, now standard across many disciplines, support much contemporary research and technology activity.

A further example of how THz technology compares unfavourably with other spectral ranges is in the context of THz microscopy and analysis below the diffraction limit, which intrinsically restricts such measurements to ensemble sampling of physical properties averaged over the size, structure, orientation and density of, for example, nanoparticles, nanocrystals or nanodomains. Although near-field imaging approaches have been adapted from the visible/infrared regions enabling THz measurements on the micro/nano-scale, no THz instrument currently provides the required spatial resolution and sensitivity, nor can address the enormous range of length-scales (spanning five orders of magnitude from electron confinement lengths (<10 nm) to the THz wavelength (~300 um)), nor can operate at cryogenic temperatures. In fact, on this point, the THz field is deficient even in the provision of basic technologies such as waveguides and coupling optics required to deliver THz signals with low loss into cryostats or industrial apparatus.

In this programme we will create the first comprehensive instrumentation for precise THz frequency spectroscopy, microscopy, and coherent control. This will be based upon our unique and proprietary capabilities to generate, and manipulate photonically, THz signals of unprecedentedly narrow (Hz) linewidth and with sub-wavelength spatial resolution. The instrumentation will then be exploited to create new challenge-led applications in non-destructive testing and spectroscopic analysis for electronics and atmospheric sensing, inter alia, as well as discovery-led opportunities within physics, quantum technologies, materials science, atmospheric chemistry and astronomy.

Planned Impact

This programme will develop new instruments for precise THz frequency spectroscopy, microscopy, and coherent control.

Economic Impact: Recent market studies predict strong growth in THz-based technologies over the next decade: e.g. Prescouter in 2015 predict that the market for current THz imaging and spectroscopy applications will grow from $127 million in 2016 to $570 million in 2021, and importantly, find that new microscopy and spectroscopy instrumentation and methodologies will accelerate this further. We will pursue a number of approaches to develop economic impact, as appropriate for the TRL level of the technology, including collaboration with existing companies to (i) transfer our technology into current commercial products, (ii) develop new commercial products, and (iii) create new companies where this will accelerate product development. Our new spectroscopy and microscopy instrumentation will provide versatile instrumentation for the scientific and R&D markets, with immediate application in non-destructive testing and spectroscopic analysis, inter alia. These include high-throughput microscopy requirements identified by Project Partner TeraView and other end-users in the testing of integrated circuits with international foundries, as well as other high-throughput THz imaging and microscopy applications in the medical, food, and pharmaceutical sectors. Longer-term economic impacts will be delivered through, for example, the applicability of our instrumentation to manipulate coherently quantum dots, and other mesoscopic electronic systems, in a compact and portable footprint. This adds capability to Project Partner Toshiba's development of single-photon and entangled-photon pair sources for applications to quantum key distribution and quantum computing, and the 'THz-to-Telecoms' bridge will lead to on-chip integrated quantum photon converters and hybrid single-photon detectors.

Knowledge Impact: We anticipate very considerable new knowledge generation in the fields of electronic engineering, condensed matter and optical physics, quantum technologies, materials science, atmospheric chemistry, inter alia, with new knowledge not only generated during the course of the Programme, but also created in the future though application of the instrumentation that we will develop. To give one example, our robust frequency-locked QCL spectroscopy systems will find application as local oscillators in satellite instrumentation for Earth-observation and planetary science, and in high-precision gas spectroscopy, and will create knowledge impact when exploited by chemists, atmospheric chemists, astronomers, and electronic engineers. Such instrumentation is necessary for future airborne and satellite-based Earth-observation missions above 2 THz, and with Project Partner DLR, we will integrate our technology onto SOFIA, a joint NASA/DLR project on a modified Boeing 747-SP aircraft to enable e.g. investigations and new knowledge of narrow-frequency outflows in shock regions of the interstellar medium. With RAL, we will address the more stringent requirements of satellite instrumentation enabling e.g. the analysis of OH (3.5 THz) and O (4.7 THz) species in the Earth's mesosphere/lower thermosphere, informing studies and new understanding of climate change, inter alia.

Societal Impact and Impact on People: THz science and technology is of national and global importance, and Society will benefit economically and through provision of new measurement and sensing instrumentation that will support high technology industry, including in the communications, non-destructive testing, and electronics sectors. We will also produce skilled People at doctoral and post-doctoral level having both technology and applications perspective, as well as developing current and future research leaders and role models.
 
Description The vision for HyperTerahertz was to open up new opportunities for the terahertz (THz) frequency range through the development of new instrumentation for precise THz spectroscopy, microscopy, and coherent control, and to prove and apply the technology in proof-of-concept studies. The five-year programme was defined by a series of formal objectives and exceptional progress has been made against each of them.

We demonstrated the first continuous-wave (cw) injection locking of a quantum cascade laser (QCL), with the QCL emission locked to a fibre-based near-infrared telecommunications frequency comb, itself referenced to a GPS-locked microwave frequency synthesiser, providing traceability of the QCL frequency to primary standards. This not only stabilizes the QCL frequency, and enables independent control of the frequency and phase for the first time, but also reduces the QCL linewidth to <1 Hz, and allows the phase-locked cw QCL emission to be detected coherently. This brings the frequency precision and accuracy available at microwave frequencies to the THz region of the spectrum for the first time, and as all components are semiconductor-based, compact integration is possible benefitting scientific application. We also demonstrated a bench-top QCL-based instrument capable of producing synchronized intense, narrowband, transform-limited pulses, with pulse lengths down to 650 ps. Sequences of twin pulses were also demonstrated where the pulse widths, delay and amplitude were independently controlled electronically. This narrowband pulse spectrometer will find application in the study of narrowband excitation and relaxation processes at THz frequencies and in coherent communications. Considerable work has furthermore been completed on packaging fibre-coupled uni-travelling-carrier photodiodes (UTC-PDs) with integrated antennas for future integrated QCL locking and high-precision spectroscopy.

We have pursued both room temperature and cryogenic near-field scanning THz microscopy, exploiting scattering- and aperture-based approaches. Our THz s-SNOM exploiting self-mixing detection, for example, was successfully integrated into a commercial platform and <30 nm resolution microscopy demonstrated. To enable the a-SNOM to image coherently and operate with cw QCL sources, we integrated semiconductor nanowire and nano-scale FET THz detectors into the probe aperture. These instruments have been applied to the investigation of samples and materials including: study of phonon-polariton-resonant crystals; imaging of localized plasmonic resonance modes in antenna structures and metamaterials; and, the study of TI materials, the latter requiring considerable aligned effort in the growth and device fabrication of these contemporary materials systems. The cryogenic microscopy programmes faced significant technical challenges caused by vibrational interference arising from the cryo-cooler compressor that affected the microscope resolution. A spring-coupled floating stage arrangement was developed with the cryo-cooler manufacturer, dramatically reducing the tip vibration, and opening the way for full cryogenic THz microscopy in future programmes.

We developed a toolkit of components including waveguides, reflectors, windows, and feedthroughs to couple THz radiation into difficult to access environments, focussing on 4.2 K and 1.5 K cryostats, and dilution refrigerators. QCL transmission within a dilution refrigerator was demonstrated, resulting in base and electron temperatures of, respectively, 109 mK and 430 mK, the latter in an InGaAs-AlGaAs two-dimensional electron system (2DES) during cyclotron absorption measurements. We also successfully designed, developed, and demonstrated antenna-coupled direct THz detectors exhibiting high responsivities, leading to the discovery of a new physical phenomenon-the in- plane photoelectric effect. And finally, excellent progress was made developing efficient large-area photoconductive array structures for generation and detection of high-power THz pulses, and in the use of these in proving work on 2D non-linear spectroscopy of the atom-in-solid material Ge:As.

The programme has demonstrated significant consortium cohesion and collaboration, with many inter-site visits for joint experiments, sample and technology transfer, and discussion. The covid-19 pandemic disruption inevitably had a negative impact on the breadth and coverage of the programme's later activities as originally envisaged, but we successfully prioritized and focussed research to maximize impact and publications. We actively pursued public understanding of science and community engagement; for example, we presented at the Royal Society Summer Science Exhibition, developed a series of YouTube videos, worked with the Royce Institute to bring together the THz microscopy and 2D materials communities, and we lead the TeraNet UK Network. Programme sustainability includes both aligned and follow-on funding ranging from new programme grants (EP/V001914/1, EP/W028921/1) and responsive mode grants (EP/T034246/1, EP/V004743/1, EP/W03252X/1), to UKRI Future Leader Fellowships (Valavanis, Balakier, Ponnampalam). The development of our diverse and talented PGR and PDRA cohort and their progress from this programme into subsequent academic and industrial positions has been a particular highlight.
Exploitation Route We have a series a further research grants, building on this programme, which are taking important aspects of this work forward. A significant output of the programme comprises our diverse team of PGR and PDRA colleagues, supported and developed during this programme, who are taking the outcomes and their skills to new positions both in academia and industry. We have actively published our work in order to disseminate the work to others, in journals and conference, as well as through industrial/KTN meetings, and in public events such as the Royal Society Summer Exhibition and BeCurious.
Sectors Aerospace

Defence and Marine

Digital/Communication/Information Technologies (including Software)

Electronics

Environment

Healthcare

Other

URL http://www.hyperterahertz.org
 
Description Although the impact to date is predominantly academic and discussed elsewhere in this submission, it is worth noting the potential nucleation of a new research methodology arising from his programme. The ability to introduce terahertz frequency radiation in to cryogenic environments would open up a platform for investigating quantum coherence and entanglement, developing new quantum computing architectures, exploring superconductivity and magnetism in novel materials, and testing many other quantum devices and sensors. The introduction of terahertz radiation from a quantum cascade laser into a mK dilution refrigerator, maintaining the sample temperature around 100 mK, as demonstrated in this programme, is now receiving interest for further instrument development and new academic collaborations.
First Year Of Impact 2022
Sector Digital/Communication/Information Technologies (including Software)
Impact Types Societal

 
Description (EXTREME-IR) - Extreme Optical Nonlinearities in 2D materials for Far-Infrared Photonics
Amount € 3,647,534 (EUR)
Funding ID 964735 
Organisation European Commission 
Sector Public
Country European Union (EU)
Start 08/2021 
End 02/2025
 
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 Coherent pulse propagation and modelocking in terahertz quantum cascade lasers
Amount £1,127,385 (GBP)
Funding ID EP/T034246/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 03/2021 
End 08/2024
 
Description Electromagnetic Environment Hub
Amount £7,000,000 (GBP)
Funding ID RQ0000010374 
Organisation Defence Science & Technology Laboratory (DSTL) 
Sector Public
Country United Kingdom
Start 01/2022 
End 12/2025
 
Description High-speed Terahertz Imaging using Rydberg Atoms & Quantum Cascade Lasers
Amount £352,308 (GBP)
Funding ID EP/W03252X/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 06/2022 
End 06/2025
 
Description Nanoscale Advanced Materials Engineering
Amount £7,671,801 (GBP)
Funding ID EP/V001914/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 06/2021 
End 06/2026
 
Description Terabotics - terahertz robotics for surgery and medicine
Amount £8,000,773 (GBP)
Funding ID EP/V047914/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 08/2021 
End 08/2026
 
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
 
Description BeCurious Science Festival (Leeds, March 2019). 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach Regional
Primary Audience Public/other audiences
Results and Impact BeCurious is the University of Leeds annual public engagement festival. We held a series of hands-on demonstrations for the general public and school children.
Year(s) Of Engagement Activity 2019
 
Description BeCurious Science Festival (on-line, Leeds, July 2021). 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Public/other audiences
Results and Impact BeCurious is the University of Leeds annual science festival. In 2021 it was held remotely owing to the pandemic restrictions. We presented three short talks, and a live experimental demonstration.
Year(s) Of Engagement Activity 2021
 
Description Industrial and end-user engagement 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Industry/Business
Results and Impact We attended and presented at the Innovate UK Showcasing Emerging Technologies 2018 - Photonics and Imaging KTN event in London in 2018. We presented a working THz QCL imaging system and discussed the application and potential of THz imaging and spectroscopy, and the HyperTerahertz programme. We also presented our work at the KTN Materials Research Exchange (MRE) also in London in 2018, 2020, and 2022.
Year(s) Of Engagement Activity 2018,2020,2022
URL https://ktn-uk.co.uk/events/showcasing-emerging-technologies-2018-photonics-and-imaging
 
Description Instructional YouTube videos 
Form Of Engagement Activity Engagement focused website, blog or social media channel
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Public/other audiences
Results and Impact We developed a series of four YouTube videos to promote our work, the field of terahertz science and technology, and our funding body EPSRC. They are stand alone and also used in conjunction with our live public engagement activities.
Year(s) Of Engagement Activity 2019
URL http://www.youtube.com/channel/UCnXnbpJKnvkYymVnc_9_Q2A
 
Description Royal Society Summer Science Exhibition (London, July 2019). 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Public/other audiences
Results and Impact A talk, presentation, and experimental demonstration at the Royal Society Summer Science Exhibition 'Lates' session.
Year(s) Of Engagement Activity 2019