EPSRC Fellowships in Manufacturing - "Manufacturing Routes for Organic Room-Temperature MASER"

Lead Research Organisation: Imperial College London
Department Name: Materials

Abstract

The aim of this fellowship is to take a recently reported discovery, namely a solid-state maser capable of operating at room temperature, and to carry out a programme of work based upon it that will enhance "manufacturability" for two key application areas.

Background:
The MASER, standing for Microwave Amplification by Stimulated Emission of Radiation, was invented some 60 years ago and exploits paramagnetic transitions in quantum systems to amplify rf/microwave signals. The LASER, which followed directly on from it a few years later, operates through exactly the same physical mechanism (namely stimulated emission) but at much higher frequencies, exploiting electronic transitions to amplify -and so generate- ultraviolet, visible, and infrared light. As devices, masers are useful because they can amplify extremely weak (often precious) electromagnetic signals without corrupting them through the addition of random noise, as would otherwise happen if noisier, conventional (semiconductor-based) amplifiers were used.

Lasers are now ubiquitous and have found their way into a plethora of applications. Masers, on the other hand, are used only in specialised, performance-critical applications such as atomic clocks or as low-noise amplifiers in the most sensitive radiofrequency telescopes and ground stations. The cause of their relative obscurity to date is that all maser systems offering useful performance have necessarily included pieces of kit that are either bulky or consume substantial amounts of power (often kilowatts), or both. Specifically, conventional solid-state masers, as developed and used by NASA, require both cryogenic temperatures and substantial applied d.c. magnetic fields to work, so in turn requiring bulky, power-consuming refrigerators and magnets. Atomic/molecular masers, though capable of room-temperature operation (after a fashion), still require bulky vacuum chambers and pumps, which are equally hard to miniaturize. The novel type of maser to be developed through this fellowship avoids these limitations: it works in air, at room temperature, in the Earth's ambient magnetic field. It is thus, in principle, vastly more amenable to cost-sensitive, portable applications.

How the Fellowship specifically adds value:

Preliminary work leading to a proof-of-principle demonstrator has now been published*, but there remain issues that substantially inhibit manufacturability:

1 The prototype works only in pulsed mode; continuous (CW) operation is sought though with thermal implications concerning the removal of waste heat.

2 Wall-plug power efficiency must to be improved, aiming to get the threshold for CW masing down to a few watts.

3 Physical miniaturisation is required for portable applications.

Substantial progress on 1, 2 and 3 can be made through engineering solutions alone (as opposed to further "breakthroughs"), whilst being ever mindful of:

4 Certain critical components are currently made out of expensive-to-grow single crystals that are equally expensive to form (by skilled hand grinding and polishing) into their required shapes. These build costs need to be extracted.

The purpose of the fellowship is to find solutions to all of the above impediments -focussing especially on the last of them 4 and allowing it to regulate the more engineering activities in 1, 2 and 3.

* Room temperature solid-state maser, M.O., J. D. Breeze & N. M. Alford, Nature, DOI 10.1038/nature11339, 16th August 2012; see also Aharon Blank's "New and Views" (ibid.): http://www.nature.com/nature/journal/v488/n7411/full/488285a.html

Planned Impact

This fellowship will bring a new type of spintronic amplifier, namely an organic maser optically pumped via molecular intersystem crossing, to a manufacturing readiness level (MRL) of 4*. The attractiveness of the device in applications stems from its operational convenience (room-temperature, ambient magnetic field) in conjunction with its superior performance over existing semiconductor amplifiers -including cryogenically operated ones- in the areas of added white noise (i.e. the amplifier's noise figure/temperature), intermodulation distortion, peak-power reserve, and 1/f ("flicker") noise. Its resultant beneficiaries include:

(1) Biochemical analysis: specifically, improved spectrometers and scanners based on magnetic resonance, i.e. EPR, NMR, ENDOR. There are actually two distinct, yet potentially combinable, forms of maser-enhancement:

(a) As explained in ref. [1], the low-noise attribute of maser amplifiers and oscillators (potentially incorporated within the EPR/NMR cavity itself) can boost sensitivity, towards detecting extremely minute amounts of a particular molecular species/marker.

(b) In so-called "multi-quantum" (MQ) EPR spectroscopy [2], the sample is exposed to two tones of microwave radiation closely separated in frequency. This obviates the need for a.c. magnetic-field modulation leading to substantial hardware simplifications. The competiveness of MQ-EPR has, however, been hampered by parasitic IM distortion of the sample's bi-tonal response introduced by semiconductor amplifiers. The far lower IM distortion of a maser obviates this problem.

(2) Security: anti-stealth RADAR, electronic warfare (EW) and countermeasures. Basically, the absence of IM makes maser receivers more difficult to jam. Also, in stark contrast to micro/nano-scale semiconductor junctions and channels, "mesoscopic" maser preamplifiers are a great deal more difficult to destroy, electromagnetically, by projected-energy weaponry.

(3) Super-resolution is difficult to achieve with passive metamaterials at microwave frequencies due to Ohmic loss in the metallic elements (e.g. split rings) within the material. Distributed maser gain allows for the realizing of active hyperlenses [3] that can overcome this problem.

(4) Space: improved communication downlinks for both micro-satellites and deep-space probes (e.g. ESA's new JUICE mission), where transmit power is severely limited. [4]

(5) Astronomy: more sensitive radio telescopes -exploiting a maser's low noise temperature, low IM, and low 1/f noise.

(6) Particle accelerators: In contrast to semiconductor devices, a maser holds a stockpile of inverted-spin energy that can be released suddenly. This enables the realization of compact microwave cavities capable of accelerating particles via the mechanism of PASER (particle acceleration by stimulated emission of radiation), as is being explored by a group associated with Argonne National Laboratory (and its wakefield accelerator) [5].

The work proposed here will impact on all of the above applications by making them affordable.

* See (for example): http://en.wikipedia.org/wiki/Manufacturing_Readiness_Level

[1] "Theoretical and experimental senstitivities of ESR spectrometers using maser techniques", J.C. Mollier et al, Rev. Sci. Instrum. 44, 1763-71(1973).

[2] "A general purpose multi-quantum electron paramagnetic resonance spectrometer", R. A. Strangeway et al, Rev. Sci. Instum 66, 4516-28 (1995).

[3] "Gain-assisted hybrid-superlens hyperlens for nano imaging", Y.-T. Wang et al, Optics Express 20, 22954 (2012)

[4] "Ruby masers", R. C. Clauss & J. S. Shell, in Low-Noise Systems in the Deep Space Network, Caltech (2008); http://descanso.jpl.nasa.gov/Monograph/series10/03_Reid_chapt+3.pdf

[5] "Photoinduced spin polarization and microwave technology", Sergey Antipov et al, Nucl. Instr. & Methods in Phys. Res. A, online 22 October 22, http://dx.doi.org/10.1016/j.nima.2012.10.016

Publications

10 25 50
publication icon
Arroo D (2021) Perspective on room-temperature solid-state masers in Applied Physics Letters

publication icon
Bogatko S (2016) Molecular Design of a Room-Temperature Maser in The Journal of Physical Chemistry C

publication icon
Breeze J (2015) Enhanced magnetic Purcell effect in room-temperature masers. in Nature communications

publication icon
Burnett J (2013) Slow noise processes in superconducting resonators in Physical Review B

publication icon
Déjean V (2020) Detection of magnetic field effects by confocal microscopy. in Chemical science

publication icon
Keyser AKV (2020) Pulsed electron spin resonance of an organic microcrystal by dispersive readout. in Journal of magnetic resonance (San Diego, Calif. : 1997)

publication icon
Lubert-Perquel D (2018) Identifying triplet pathways in dilute pentacene films. in Nature communications

publication icon
Mihalkovic M (2014) Ab-initio tiling and atomic structure for decagonal ZnMgY quasicrystal in Philosophical Magazine

 
Description How to construct chip-scale solid-state masers capable of operating at room temperature.
How to construct luminescent concentrators suitable for vascular skin surgery and cosmetic treatments.
Both of these advances are patent-protected breakthroughs leading to new gadgets, services and jobs for the benefit of the UK's economy.
Exploitation Route Commercialization, spin-outs and/or licensing
Sectors Aerospace, Defence and Marine,Chemicals,Digital/Communication/Information Technologies (including Software),Electronics,Environment,Healthcare,Manufacturing, including Industrial Biotechology,Pharmaceuticals and Medical Biotechnology,Security and Diplomacy

 
Description The research has been exploited in two areas: [1] A UK-RI funded team based in Cornwall are now exploiting designs and know-how developed through the project to develop extremely high-powered microwave resonators for pest control without insecticides or GM. See: https://gtr.ukri.org/projects?ref=99116 . As off Spring 2022, this is now a very active thread of research/innovation. First field trials at Harper Adams University in the Summer of 2022. (See collaborations and partners). [2] Separate know-how developed during the project was used to develop a new type of intense yellow light source (luminescent concentrator). This thread stalled around 2019 due to lack of UK (commercial) funding/interest. Still being developed by Philips in the Netherlands for mercury-free video projectors.
First Year Of Impact 2019
Sector Aerospace, Defence and Marine,Agriculture, Food and Drink,Chemicals,Healthcare,Security and Diplomacy
Impact Types Societal,Economic

 
Title Cambridge Structure Database 
Description The structures of various organic molecular crystals and co-crystals have been added (by PDRA Riccardo Montis) to the CSD. One example is the co-crystal comprising pentacene and dihydropentacene. These crystals were (some still are) candidates for maser action at room temperature. 
Type Of Material Database/Collection of data 
Year Produced 2017 
Provided To Others? Yes  
Impact None yet. 
URL https://www.ccdc.cam.ac.uk/solutions/csd-system/components/csd/
 
Description A*Star (Singapore) Secondee 
Organisation Agency for Science, Technology and Research (A*STAR)
Country Singapore 
Sector Public 
PI Contribution Training of A*Star Secondee.
Collaborator Contribution Ke-Jie Tan, a research fellow externally sponsored by A*Star worked full time on the growth of maser crystals in our laboratory at Imperial from the summer of 2013 to the summer of 2015. He is now back at A*Star doing related work (on organic semiconductors).
Impact Supply of high-quality organic crystals to other research group in the UK, e.g. Peter Hore and Christiane Timmel at Oxford University Poster presentation about the growth of maser crystals at 2014 MRS Fall Meeting in Boston.
Start Year 2013
 
Description Optically excited pulsed EPR facility at UCL (Chris Kay) 
Organisation University College London
Department Division of Biosciences
Country United Kingdom 
Sector Academic/University 
PI Contribution Supply of materials, equipment and know-how for the demonstration of room-temperature solid-state masing at UCL. This has included: Bespoke synthesis and deuteration of candidate maser molecules Growth of molecular crystals by Bridgman and solution-growth methods Characterization of same using UV-Vis, x-ray, SIMMS ... Supply of maser crystal, microwave cavities and associated instrumentation Providing consultancy on interpretation of results.
Collaborator Contribution Access and operation of pulse-EPR spectrometer
Impact High multi-disciplinary, spanning EPR spectroscopy Molecular crystal growth and characterization Low-noise microwave instrumentation Optical (laser) metrology: spectra, power/energy, polarization of optical light sources.
Start Year 2013
 
Description RF magnetic induction pest controller for cabbage stem flea beetle control - commercial prototype 
Organisation Harper Adams University
Country United Kingdom 
Sector Academic/University 
PI Contribution The application area here is the killing of certain pests, e.g. cabbage stem flea beetle, which is currently devastating the UK's oil-seed rape crops, without using chemical insecticides and/or resorting to genetic modifications (GM). This application might seem light years away from low-noise microwave amplification with masers but the skills and know-how needed to design an efficient, effective maser are exactly the same as those that are needed to design high-power dielectric resonators working at hundreds of watts (or even kilowatts) for pest control. Hence the technology transfer from "masers" to "insect/grub zappers". I am now collaborating with a Cornwall-based consortium (labs located at ESAM, near St. Austell) to develop demonstrators and prototypes or the technology: resonators that lethally expose insects to intense magnetic fields at GHz frequencies that leave the leaves, flowers and grains of plants unscathed. Contributions (work packages in the project): (a) RF consultancy towards defining novel design of developed microwave resonator for killing crop-destroying pests. (b) Metrology: development of novel probe (based on a temperature-sensitive liquid crystal) to measure strength of the high-frequency magnetic fields used.
Collaborator Contribution None. Technology/know-how transfer from academia to industry.
Impact Novel design of microwave resonator for killing agricultural pests without the need for insecticides or GM. Novel design of magnetic field probe at microwave frequencies.
Start Year 2021
 
Description Supply of zone-refined anthracene and tetracene cystals 
Organisation University of Oxford
Department Radcliffe Department of Medicine
Country United Kingdom 
Sector Academic/University 
PI Contribution Post-docs Ke-Jie Tan and Riccardo Montis supplied Peter Hore and Christiane Timmel's groups in Oxford (Chemistry) with samples of anthracene and tetracene crystals which they themselves were not set up to grow. These gifts helped their research.
Collaborator Contribution None.
Impact The main results reported in PhD student Jennifer Handsel's thesis we made on Imperial-grown specimens
Start Year 2015
 
Description VERY YELLOW: An Intense Yellow Light Source for Clinical and Cosmetic Skin Surgery 
Organisation Derm-appeal
Country Netherlands 
Sector Private 
PI Contribution I/we have provided the key ideas and demonstrators (covered by patents) for a novel, non-laser light source suitable for both cosmetic skin treatments and vascular skin surgery. These treatments are currently provided by liquid-dye lasers, which are hazardous (the dye solution is both flammable and carcinogenic) and require regular maintenance. The new source was originally developed as an efficient pump source for optically-pumped masers based on pentacene-doped para-terphenyl (which absorbs yellow light), but I am now exploiting the same technology for a different -and, potentially, a rather more immediately lucrative-- application.
Collaborator Contribution Protected through an NDA, the collaboration currently comprises myself and: [1] a small London-based firm, Photronics Ltd, who specialize in the servicing of cosmetic lasers and who have first-hand knowledge of the UK's market for clinical/cosmetic laser treatments. The person principally involved from this company is Dr. Simon Rondell. http://www.photronics.co.uk/ Dr. Rondell has supplied machines and instrumentation for testing the performance of prototypes. [2] a Dutch company, Dermappeal, who have experience in commercializing products in the clinical and personal beauty sector, incl. gaining FDA approval and CE accreditation. http://www.dermappeal.nl/ The person principally involved from this company is Ralf van Gogh, who has supplied advice on commercialization. [3] Imperial Innovations (viz Brian Graves, et alia).
Impact Prototypes/demonstrators for commercial exploitation --still in pre-patent stealth mode (they will be the described "embodiments" in the patent filing). The collaboration involves the following disciplines: crystal growth, laser physics, biophysics (interaction of light with human skin/flesh), production technologies (cutting, grinding polishing, assembly), commercialization: market assessment, trials, patenting, documentation/protocols.
Start Year 2015
 
Description VERY YELLOW: An Intense Yellow Light Source for Clinical and Cosmetic Skin Surgery 
Organisation Photronics Ltd
Country United Kingdom 
Sector Private 
PI Contribution I/we have provided the key ideas and demonstrators (covered by patents) for a novel, non-laser light source suitable for both cosmetic skin treatments and vascular skin surgery. These treatments are currently provided by liquid-dye lasers, which are hazardous (the dye solution is both flammable and carcinogenic) and require regular maintenance. The new source was originally developed as an efficient pump source for optically-pumped masers based on pentacene-doped para-terphenyl (which absorbs yellow light), but I am now exploiting the same technology for a different -and, potentially, a rather more immediately lucrative-- application.
Collaborator Contribution Protected through an NDA, the collaboration currently comprises myself and: [1] a small London-based firm, Photronics Ltd, who specialize in the servicing of cosmetic lasers and who have first-hand knowledge of the UK's market for clinical/cosmetic laser treatments. The person principally involved from this company is Dr. Simon Rondell. http://www.photronics.co.uk/ Dr. Rondell has supplied machines and instrumentation for testing the performance of prototypes. [2] a Dutch company, Dermappeal, who have experience in commercializing products in the clinical and personal beauty sector, incl. gaining FDA approval and CE accreditation. http://www.dermappeal.nl/ The person principally involved from this company is Ralf van Gogh, who has supplied advice on commercialization. [3] Imperial Innovations (viz Brian Graves, et alia).
Impact Prototypes/demonstrators for commercial exploitation --still in pre-patent stealth mode (they will be the described "embodiments" in the patent filing). The collaboration involves the following disciplines: crystal growth, laser physics, biophysics (interaction of light with human skin/flesh), production technologies (cutting, grinding polishing, assembly), commercialization: market assessment, trials, patenting, documentation/protocols.
Start Year 2015
 
Title Ce:YAG Luminescence concentrator 
Description A light source made in house for optically pumping maser crystals is being exploited by clinicians for cosmetic skin surgery.The light source is based on luminescent/fluorescence concentration in bars of cerium-doped YAG. This patent covers our first most basic design. 
IP Reference US20170329065 
Protection Patent application published
Year Protection Granted 2017
Licensed No
Impact A "spin-out" collaboration involving an established London (Enfield)-based SME that services medical lasers has been forged.
 
Title Luminescent concentrator 
Description Extremely bright and efficient solid-state source of yellow light. Applications include: skin surgery/beauty therapies and colour video projectors. 
IP Reference P61579GB 
Protection Patent application published
Year Protection Granted 2014
Licensed No
Impact This patent protects the collaboration with Photronics Ltd, Derm-appeal and Imperial Innovations (mentioned in the collaborations section) towards commercializing the luminescent concentrator technology.
 
Title MASER ASSEMBLY 
Description A maser assembly includes a pump light source; a maser material including molecules that are excited through the absorption of light (1) from the pump light source, and which subsequently transfer via intersystem crossing (9) into the sublevels of their triplet ground states, so causing a population inversion between two sublevels (16,18); an electromagnetic structure in which the masing material is disposed, and which supports a microwave mode that is both resonant in frequency with and magnetically coupled to the transition between these two sublevels; and where energy is supplied to the microwave mode through stimulated emission (25) across the transition at such a rate as to exceed the mode's electromagnetic losses, the microwave mode being a maser mode. The assembly includes provisions for effecting substantially continuous maser activity during operation of the assembly. The laser crystal may be a (perdeuterated) pentacene in p-terphenyl which is held at room temperature without an additional magnetic field and the dye molecules in the single crystal may be pumped by blue LED with a frequency conversion to the yellow and green with the help of a Ce:YAG fluorescent pump light concentrator. 
IP Reference US2015214687 
Protection Patent granted
Year Protection Granted 2015
Licensed No
Impact None yet.
 
Title MASER ASSEMBLY 
Description A maser assembly includes a pump light source; a maser material including molecules that are excited through the absorption of light from the pump light source, and which subsequently transfer via intersystem crossing (ISC) into the sublevels of their triplet ground states, so causing a population inversion between two sublevels of same; an electromagnetic structure in which the masing material is disposed, and which supports a microwave mode that is both resonant in frequency with and magnetically coupled to the transition between these two sublevels; and where energy is supplied to the microwave mode through stimulated emission across the transition at such a rate as to exceed the mode's electromagnetic losses, the microwave mode being a maser mode. The assembly includes provisions for effecting substantially continuous maser activity during operation of the assembly. 
IP Reference WO2014027205 
Protection Patent granted
Year Protection Granted 2014
Licensed Commercial In Confidence
Impact Ongoing commercialization through Imperial Innovations
 
Title Novel light source for both vascular surgery and cosmetic skin treatments based on the principle of luminescent concentration 
Description A series of lab demonstrators have been developed testing design principles --towards improving the directivity and wall-plug efficiency of the light source. The device has been tested on the skin of "volunteers". human skin. 
Type Therapeutic Intervention - Surgery
Current Stage Of Development Initial development
Year Development Stage Completed 2017
Development Status Under active development/distribution
Impact It's early days. A team is being formed around the invention involving a London-based SME. 
 
Title 2.5D Simulation of Whispering Gallery Modes 
Description A set of macros/models working with COMSOL multiphysics for calculating, at high numerical efficiency, the frequencies and mode pattern of electromagnetic mode within ax-symmetric resonator/cavities. Most advantageously for the calculation of whispering gallery modes. 
Type Of Technology Webtool/Application 
Year Produced 2011 
Impact The simulation macros have been used extensively by both academics and industrial engineers; the research paper that launched the simulation package has been cited more than 225 times --giving some indication of the extent. Support on using the macros (this generally takes the form of answering e-mailed question received) is still on going (in 2017). 
URL https://sites.google.com/site/axisymmetricmarkoxborrow/