Showing posts with label Keith A. Nelson. Show all posts
Showing posts with label Keith A. Nelson. Show all posts

Monday, June 24, 2019

Abstract-Terahertz field–induced ferroelectricity in quantum paraelectric SrTiO3


  1. Xian Li,  
  2. Tian Qiu, 
  3. Jiahao Zhang,  
  4. Edoardo Baldini,  
  5. Jian Lu,  
  6. Andrew M. Rappe
  7. Keith A. Nelson, 

https://science.sciencemag.org/content/364/6445/1079

“Hidden phases” are metastable collective states of matter that are typically not accessible on equilibrium phase diagrams. These phases can host exotic properties in otherwise conventional materials and hence may enable novel functionality and applications, but their discovery and access are still in early stages. Using intense terahertz electric field excitation, we found that an ultrafast phase transition into a hidden ferroelectric phase can be dynamically induced in quantum paraelectric strontium titanate (SrTiO3). The induced lowering in crystal symmetry yields substantial changes in the phonon excitation spectra. Our results demonstrate collective coherent control over material structure, in which a single-cycle field drives ions along the microscopic pathway leading directly to their locations in a new crystalline phase on an ultrafast time scale.

Wednesday, April 25, 2018

US PATENT-Systems, apparatus, and methods of nonlinear terahertz (THz) magnetic resonance measurement


United States Patent 9945914
Inventors:
Hwang, Harold Young (Cambridge, MA, US) 
Lu, Jian (Medford, MA, US) 
Zhang, Yaqing (Cambridge, MA, US) 
Ofori-okai, Benjamin K. (Cambridge, MA, US) 
Nelson, Keith A. (Newton, MA, US) 
Li, Xian (Cambridge, MA, US) 

http://www.freepatentsonline.com/9945914.html

A nonlinear terahertz (THz) spectroscopy technique uses a sample illuminated by two THz pulses separately. The illumination generates two signals Band BB, corresponding to the first and second THz pulse, respectively, after interaction with the sample. The interaction includes excitation of at least one ESR transition in the sample. The sample is also illuminated by the two THz pulses together, with an inter-pulse delay τ, generating a third signal BAB. A nonlinear signal BNL is then derived via BNL=BAB−BA−BB. This nonlinear signal BNL can be then processed (e.g., Fourier transform) to study the properties of the sample.

Monday, January 29, 2018

Abstract-Two-Dimensional Spectroscopy at Terahertz Frequencies


Jian Lu, Xian Li, Yaqing Zhang, Harold Y. Hwang, Benjamin K. Ofori-Okai, Keith A. Nelson

https://link.springer.com/article/10.1007%2Fs41061-018-0185-4

Multidimensional spectroscopy in the visible and infrared spectral ranges has become a powerful technique to retrieve dynamic correlations and couplings in wide-ranging systems by utilizing multiple correlated light-matter interactions. Its extension to the terahertz (THz) regime of the electromagnetic spectrum, where rich material degrees of freedom reside, however, has been progressing slowly. This chapter reviews some of the THz-frequency two-dimensional (2D) spectroscopy techniques and experimental results realized in recent years. Examples include gas molecule rotations, spin precessions in magnetic systems, and liquid molecular dynamics studied by 2D THz or hybrid 2D THz-Raman spectroscopy techniques. The methodology shows promising applications to different THz-frequency degrees of freedom in various chemical systems and processes.

Friday, October 27, 2017

Keith Nelson awarded the Frank Isakson Prize for Optical Effects in Solids



The Izakson Prize is given in recognition of outstanding optical research that leads to breakthroughs in the condensed matter sciences.

Danielle Randall
http://news.mit.edu/2017/keith-nelson-awarded-frank-isakson-prize-optical-effects-solids-1023

The American Physical Society has selected Haslam and Dewey Professor of Chemistry Keith A. Nelson as the recipient of the 2018 Frank Isakson Prize for Optical Effects in Solids. Nelson was chosen by the award's selection committee for pioneering contributions to the development and application of ultra-fast optical spectroscopy to condensed matter systems, and providing insight into lattice dynamics, structural phase transitions, and the non-equilibrium control of solids.
“[This award] is very special for me, because a great deal of the progress in my research into molecular and collective dynamics has been enabled by discoveries of new light-matter interactions, in most cases demonstrated first in crystalline solids and then in liquids and isolated molecules,” Nelson said. “The optical effects themselves are fascinating to me, and it’s deeply gratifying to see them recognized.”
The Isakson Prize is awarded biennially (in even-numbered years) as a memorial to Frank Isakson. It  is given in recognition of outstanding optical research that leads to breakthroughs in the condensed matter sciences. The prize, which consists of $5,000, as well as a certificate citing Nelson’s contributions, will be presented to him at the meeting of the American Physical Society. The award was established in 1979, and supported by the Photoconductivity Conference. Since 1994, it has been supported by Solid State Communications.
Nelson’s research interests are in ultrafast optics, coherent spectroscopy, and coherent control over collective dynamics and structure in condensed matter. He has worked on discovery of new light-matter interactions and their exploitation for spectroscopy and control of coherent acoustic waves, lattice and molecular vibrations, excitons, spins, and their admixtures with light. He has developed novel methods for study of solid-state chemical reactions, crystals near phase transitions, glass-forming liquids, electronic excited-state dynamics, thermal transport, and matter far from equilibrium. Nelson has pioneered tabletop generation of strong terahertz frequency fields and nonlinear terahertz spectroscopy.

Wednesday, August 9, 2017

Abstract-Terahertz-driven Luminescence and Colossal Stark Effect in CdSe:CdS Colloidal Quantum Dots


Brandt PeinWendi ChangHarold Young HwangJennifer M SchererIgor CoropceanuXiaoguang ZhaoXin ZhangVladimir BulovicMoungi G. Bawendi, and Keith A. Nelson

http://pubs.acs.org/doi/abs/10.1021/acs.nanolett.7b01837?mi=aayia761&af=R&AllField=nano&target=default&targetTab=std

Optical properties of colloidal semiconductor quantum dots (QDs), arising from quantum mechanical confinement of charge, present a versatile testbed for the study of how high electric fields affect the electronic structure of nanostructured solids. Studies of quasi-DC electric field modulation of QD properties have been limited by electrostatic breakdown processes under high externally applied electric fields, which have restricted the range of modulation of QD properties. In contrast, here we drive CdSe:CdS core:shell QD films with high-field THz-frequency electromagnetic pulses whose duration is only a few picoseconds. Surprisingly, in response to the THz excitation we observe QD luminescence even in the absence of an external charge source. Our experiments show that QD luminescence is associated with a remarkably high and rapid modulation of the QD bandgap, which changes by more than 0.5 eV (corresponding to 25% of the unperturbed bandgap energy). We show that these colossal energy shifts can be explained by the quantum confined Stark effect even though we are far outside the regime of small field-induced shifts in electronic energy levels. Our results demonstrate a route to extreme modulation of material properties and to a compact, high-bandwidth THz detector that operates at room temperature.

Friday, May 26, 2017

Abstract-Coherent Two-Dimensional Terahertz Magnetic Resonance Spectroscopy of Collective Spin Waves


Jian Lu, Xian Li, Harold Y. Hwang, Benjamin K. Ofori-Okai, Takayuki Kurihara, Tohru Suemoto, and Keith A. Nelson


We report a demonstration of two-dimensional (2D) terahertz (THz) magnetic resonance spectroscopy using the magnetic fields of two time-delayed THz pulses. We apply the methodology to directly reveal the nonlinear responses of collective spin waves (magnons) in a canted antiferromagnetic crystal. The 2D THz spectra show all of the third-order nonlinear magnon signals including magnon spin echoes, and 2-quantum signals that reveal pairwise correlations between magnons at the Brillouin zone center. We also observe second-order nonlinear magnon signals showing resonance-enhanced second-harmonic and difference-frequency generation. Numerical simulations of the spin dynamics reproduce all of the spectral features in excellent agreement with the experimental 2D THz spectra.
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Sunday, March 5, 2017

Abstract-Rapid and Precise Determination of Absolute Zero-Field Splittings by Terahertz Time-Domain Electron Paramagnetic Resonance Spectroscopy




Zero field splitting (ZFS) parameters are fundamentally tied to the geometries of metal ion complexes. Despite their critical importance for understanding the magnetism and spectroscopy of metal complexes, they are not routinely available through common techniques, and are often inferred from magnetism data or from high-field electron paramagnetic resonance (EPR) experiments. Here we demonstrate a simple tabletop experimental setup that enables direct and reliable determination of ZFS parameters at variable temperature. We report time-domain measurements of EPR associated with terahertz-frequency ZFS in molecular complexes of high-spin transition metal ions. We measure the temporal electric field profiles of the free-induction decays of spin resonances in the complexes in the absence of external magnetic fields, and we derive the EPR spectra via numerical Fourier transformation of the time-domain signals. The ZFS parameters are extracted from the measured spin resonance frequencies, and show good agreement with values obtained by other methods. The simplicity of the method portends wide applicability in chemistry, biology and material science.

Thursday, October 20, 2016

Abstract-Nonlinear two-dimensional terahertz photon echo and rotational spectroscopy in the gas phase


  1. Keith A. Nelsona,1

Molecular rotations of small molecules provide a useful testbed for examining light−matter interactions with quantum mechanical systems, but the methods of modern spectroscopy have been largely unavailable in the terahertz frequency range where most of the rotational states that are thermally populated at ordinary temperatures absorb light. Applying a pair of strong terahertz pulses, we excite molecular rotations coherently, interrogate thermally populated rotational states, manipulate the rotational motions nonlinearly, and observe connections between different rotational states spectroscopically. The method is applicable to polar molecules in flames and other reactive conditions, and it enables enhanced control over molecular motion with light.

Wednesday, October 12, 2016

Abstract-Photo-excited charge carriers suppress sub-terahertz phonon mode in silicon at room temperature


http://www.nature.com/articles/ncomms13174

There is a growing interest in the mode-by-mode understanding of electron and phonon transport for improving energy conversion technologies, such as thermoelectrics and photovoltaics. Whereas remarkable progress has been made in probing phonon–phonon interactions, it has been a challenge to directly measure electron–phonon interactions at the single-mode level, especially their effect on phonon transport above cryogenic temperatures. Here we use three-pulse photoacoustic spectroscopy to investigate the damping of a single sub-terahertz coherent phonon mode by free charge carriers in silicon at room temperature. Building on conventional pump–probe photoacoustic spectroscopy, we introduce an additional laser pulse to optically generate charge carriers, and carefully design temporal sequence of the three pulses to unambiguously quantify the scattering rate of a single-phonon mode due to the electron–phonon interaction. Our results confirm predictions from first-principles simulations and indicate the importance of the often-neglected effect of electron–phonon interaction on phonon transport in doped semiconductors.

Wednesday, October 5, 2016

Abstract-Nonlinear two-dimensional terahertz photon echo and rotational spectroscopy in the gas phase


  1. Keith A. Nelsona,1
  1. Edited by Michael D. Fayer, Stanford University, Stanford, CA, and approved September 2, 2016 (received for review June 15, 2016)

Molecular rotations of small molecules provide a useful testbed for examining light−matter interactions with quantum mechanical systems, but the methods of modern spectroscopy have been largely unavailable in the terahertz frequency range where most of the rotational states that are thermally populated at ordinary temperatures absorb light. Applying a pair of strong terahertz pulses, we excite molecular rotations coherently, interrogate thermally populated rotational states, manipulate the rotational motions nonlinearly, and observe connections between different rotational states spectroscopically. The method is applicable to polar molecules in flames and other reactive conditions, and it enables enhanced control over molecular motion with light.

Monday, May 23, 2016

Abstract-Two-dimensional terahertz magnetic resonance spectroscopy of collective spin waves



Nonlinear manipulation of nuclear and electron spins is the basis for all advanced methods in magnetic resonance including multidimensional nuclear magnetic and electron spin resonance spectroscopies, magnetic resonance imaging, and in recent years, quantum control over individual spins. The methodology is facilitated by the ease with which the regime of strong coupling can be reached between radiofrequency or microwave magnetic fields and nuclear or electron spins respectively, typified by sequences of magnetic pulses that control the magnetic moment directions. The capabilities meet a bottleneck, however, for far-infrared magnetic resonances characteristic of correlated electron materials, molecular magnets, and proteins that contain high-spin transition metal ions. Here we report the development of two-dimensional terahertz magnetic resonance spectroscopy and its use for direct observation of the nonlinear responses of collective spin waves (magnons). The spectra show magnon spin echoes and 2-quantum signals that reveal pairwise correlations between magnons at the Brillouin zone center. They also show resonance-enhanced second-harmonic and difference-frequency signals. Our methods are readily generalizable to multidimensional magnetic resonance spectroscopy and nonlinear coherent control of terahertz-frequency spin systems in molecular complexes, biomolecules, and materials.

Thursday, August 20, 2015

Abstract-Tunable multi-cycle THz generation in organic crystal HMQ-TMS


Jian Lu,1 Harold Y. Hwang,1 Xian Li,1 Seung-Heon Lee,2 O-Pil Kwon2 and Keith A. Nelson1,*

 1 Deartment of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA 2 Department of Molecular Science and Technology, Ajou University, Suwon 443-749, South Korea * kanelson@mit.edu

Abstract: We report on the generation of continuously tunable multi-cycle THz pulses with center frequencies from 0.3 to 0.8 THz in the organic nonlinear crystal, HMQ-TMS [2-(4-hydroxy-3-methoxystyryl)-1- methylquinolinium 2,-4,-6-trimethylbenzenesulfonate], by collinearly phase matched optical rectification of temporally shaped 800 nm pulses. The generation of harmonic frequency components inherent in the pulse shaper is selectively suppressed by varying the generation crystal thickness. THz pulses generated from HMQ-TMS show up to 20 times higher pulse energies compared to the benchmark inorganic THz generator ZnTe under identical conditions. The THz energy conversion efficiencies are measured to be on the order of 10−5 .


©2015 Optical Society of America OCIS codes: (160.4890) Organic materials; (190.0190) Nonlinear optics; (300.6495) Spectroscopy, terahertz. 

Thursday, June 12, 2014

Abstract-A review of non-linear terahertz spectroscopy with ultrashort tabletop-laser pulses


DOI:
10.1080/09500340.2014.918200
Harold Y. Hwang, Sharly Fleischer, Nathaniel C. Brandt, Bradford G. Perkins Jr., Mengkun Liu, Kebin Fan, Aaron Sternbach, Xin Zhang, Richard D. Averitt & Keith A. Nelson,
http://www.tandfonline.com/doi/abs/10.1080/09500340.2014.918200?journalCode=tmop20#.U5nYW5RdV8E

Over the past decade, breakthroughs in the generation and control of ultrafast high-field terahertz (THz) radiation have led to new spectroscopic methodologies for the study of light-matter interactions in the strong-field limit. In this review, we will outline recent experimental demonstrations of non-linear THz material responses in materials ranging from molecular gases, to liquids, to varieties of solids – including semiconductors, nanocarbon, and correlated electron materials. New insights into how strong THz fields interact with matter will be discussed in which a THz field can act as either a non-resonant electric field or a broad bandwidth pulse driving specific resonances within it. As an emerging field, non-linear THz spectroscopy shows promise for elucidating dynamic problems associated with next generation electronics and optoelectronics, as well as for demonstrating control over collective material degrees of freedom.

Friday, May 2, 2014

Presentation-Nonlinear terahertz spectroscopy and coherent control in solid, liquid, and gas phases


Seminar
Chemistry
Speaker:Keith Nelson
Professor of Chemistry
MIT
Nonlinear terahertz spectroscopy and coherent control in solid, liquid, and gas phases
Friday, May 30, 2014
4:00 PM  to 5:00 PM
180  Dell Butcher Hall
Rice University
6100 Main St
Houston, Texas, USA

It has recently become possible to generate single-cycle or multiple-cycle electromagnetic fields in the 1-THz frequency range with electric field strengths in the 0.1-10 MV/cm range under various conditions. This is sufficient to induce nonlinear responses in many systems including inorganic and organic crystalline solids and molecular liquids and gases. In some systems the THz field resonantly drives low-frequency electronic, lattice vibrational, or molecular rotational modes. In others, the responses are driven through nonresonant light-matter interactions including above-threshold ionization and classical acceleration of electrons to multi-eV energies. The results enable spectroscopy and control of newly accessible nonequilibrium states. High-field THz generation and interactions with different samples will be reviewed, and then two systems will be discussed in greater detail. Results from the first THz-induced phase transition, the insulator-metal transition in the prototype correlated electron system vanadium dioxide, will be presented. The collective electronic transition was monitored using THz and optical probe fields, and the coupled structural phase transition was observed through femtosecond x-ray diffraction off the crystal lattice. Finally, THz excitation of molecular rotational coherences and populations, including unique examples of field-free molecular orientation, multiple-transition coherent control, two-dimensional spectroscopy, and super(duper)radiance will be discussed.

Tuesday, January 7, 2014

MIT-Keith A. Nelson Advanced spectroscopy techniques


                                          MIT Chemistry Professor Keith A. Nelson 
                                                                                     DENIS PAISTE, MATERIALS PROCESSING CENTERhttp://web.mit.edu/newsoffice/2013/faculty-highlight-keith-a-nelson.html
Spectroscopy techniques demonstrate ballistic motion at micron length scales, open door to new possibilities for semiconductors, thermoelectrics.
Denis Paiste
Materials Processing Center

Advanced spectroscopy techniques developed by MIT Chemistry Professor Keith A. Nelson are yielding insights into heat transfer in crystalline materials that overturn long-held assumptions.

Nelson’s work could lead to the engineering of materials with tailored heat-transfer properties for use in semiconductors, thermoelectrics, and other applications where managing heat is important.


When heat travels through a solid, it is carried by acoustic phonons, which are the individual quanta of energy in an acoustic wave, just as photons are for a light wave. Phonon travel is limited by the speed of sound, which is 10,000 times slower than the speed of light. Acoustic waves for heat transport — in the range of 0.1 to 10 terahertz — are millions of times higher than the range of human hearing.

But Nelson and colleagues have developed time-resolved optical spectroscopy methods for measuring the acoustic waves associated with heat transfer.

Alternating heated and unheated regions

The technique crosses two laser beams to form an interference "grating" pattern that creates alternating heated and unheated sections in the target material. Heat from absorption of the crossed laser beams expands the material in the grating pattern, which allows the pattern to diffract probe laser light, so measurement of the diffracted signal detects the spatially varying temperature changes.

"The material is less dense where it was heated because it expanded, and there was some contraction because of that in the unheated regions, so the density now is modulated with the exact same pattern,” Nelson says. Thermal transport from the heated to the unheated regions washes out the pattern, so a gradual time-dependent decay of diffracted signal is observed. For a pattern with a particular spatial period, the measurement reveals how long heat transfer takes.

A collaborative effort through the MIT-based Solid State Solar Thermal Energy Conversion Center (S3TEC, a DOE-funded Energy Frontier Research Center) that included staff scientist Alexei Maznev and fourth-year chemistry graduate student Jeffrey K. Eliason demonstrated experimentally that in silicon at room temperature, the long-held diffusive model of heat transfer was invalid for small distances from 1 to 5 microns, where ballistic movement seems to be the driving force. (See related article.)

Random walk vs. ballistic transport

The old model was based on the assumption that phonons diffuse in a solid the way that molecules of a spray from a perfume bottle disperse in air. “By the time it gets to you several feet away, the molecules from the bottle did not go directly from the bottle to your nose in a straight unwavering path,” Nelson explains. “They got diverted and bounced back and forth all over the place, and they managed to scatter and randomly drift over to you. That’s what leads to the motion that we call diffusion.” The phenomenon is also known as random walking. Similarly, scientists had thought heat transport in a solid was governed by thermal diffusion. That assumption was based on an average phonon mean free path in silicon of about 40 nanometers.

“But it turns out when we made measurements of the thermal transport, and this was in crystalline silicon, at room temperature, later in gallium arsenide, even above room temperature, that’s not what we see,” Nelson says. Instead, the researchers saw what looked like a significant component of straight-line, ballistic motion. “Once we start getting to 20, 15, 10 microns, 5 microns, that stops, and what’s happening is, at those length scales, we no longer have purely diffusional motion. And what that’s telling us is that the things that are carrying the heat, which are these acoustic waves, are not scattering lots and lots of times, on that length scale. They’re moving ballistically.”

“That may seem like a short distance, but that’s macroscopic,” Nelson says. “I can see it in a microscope. It’s not nanometers, and in particular, when we build devices, we worry about how transport works. In materials like thermoelectrics, we care about motion on length scales like that. So we can’t model it as diffusion. The thermal conductivity that we would get is really way off if we try to do that.”

Directly measuring acoustic phonon mean free paths

Nelson hopes to directly measure the acoustic phonon mean free paths by optically generating acoustic waves and monitoring them. “We’re working hard to be able to measure acoustic waves at the highest frequencies, these terahertz-frequency acoustic waves, in different materials for this thermal transport work, and it’s hard,” Nelson says. “We don’t have very good ways of using our excitation light and turning it into terahertz-frequency acoustic waves. We’re pretty good at megahertz and gigahertz frequencies, not these highest frequencies and shortest wavelengths.” He hopes to take terahertz-frequency light waves, convert them into terahertz-frequency acoustic waves, then reconvert the terahertz-frequency acoustic wave to a terahertz-frequency light wave, and detect that. “We’re not there yet; we’re close,” he says.

Those next steps will require extremely flat interfaces and high frequencies, because the wavelengths involved will only be as short as the thickness of the interface where it happens, Nelson says. “If I have an atomically flat interface, which I can get in some materials, then I can make the very shortest acoustic wavelengths — only a couple of unit cells in length. That’s what we’re trying to do and hoping that we’ll be able to do. And it’s really only possible because we now have strong enough terahertz electromagnetic waves that we have real hope of first converting them into acoustic waves — the efficiency of that isn’t high — then reconverting those back into terahertz electromagnetic waves, again for which the efficiency isn’t high, and still detecting that at the end of the day. If I want that to work, I’d better start with a fairly strong terahertz wave, so that that weak terahertz wave I have at the end is still detectable. I think we have what we need in order to make that happen.”

Reaching out to high schools

Nelson also leads an outreach program to area high school students, the Lambda Project, which brings groups of four students at a time to the spectroscopy lab for three days. Students learn how a thin-film sample is made by deposition in the Center for Materials Science and Engineering. They also learn how to operate the spectroscopy equipment, take measurements, and analyze the data. Swampscott High School teacher Jill Sewell currently is lab manager for the program. (See related article.)

“There is a sound wave, and there’s thermal expansion, and students measure it,” Nelson says. “At a more basic level, they’re learning about nanometers and microns, for the nanometer-thickness films and micron interference spacing and so forth, and they’re learning about picoseconds and nanoseconds. For a high school student, what these length and time scales are, and what sorts of things happen or are built on those time scales or length scales, are new. There is a lot of basic learning through exposure to things they are not normally seeing.”

Sunday, September 29, 2013

The Keith Nelson Group-Terahertz polaritonics



THz Generation, Control and Detection on a Chip


Benjamin Ofori-Okai, Prasahnt Sivarajah, and Stephanie Teo

The Polaritonics platform

Terahertz (THz) radiation is the part of the electromagnetic spectrum that lies between the infrared and microwave, and it is typically associated with frequencies between 0.1 - 10 THz  (wavelength: 30 - 3000 um, energy: 3 - 300 cm-1 = 0.4 - 40 meV).  THz radiation is an important tool in basic science because it can be used to interrogate many THz-frequency phenomena including molecular rotations in a gas, vibrations in a molecular crystal (like sugar), and electronic transitions in nanostructures such as quantum wells or quantum dots.  It can also be used to probe a variety of more exotic condensed phase phenomena including Cooper pairs, polarons, and magnons. In addition, THz is has practical applications as it is the frontier in high-speed electronics, and may prove useful as a replacement for x-ray scanners in airports.
THz frequencies lie above what is easily accessible with fast electronics and below what is easily accessible with tunable lasers, so THz technology is less advanced than in other regions of the electromagnetic spectrum.  There are many challenges associated with generating and detecting THz radiation, and typically expensive ultrafast lasers are required.  Guiding the THz is also difficult: wires cannot carry high enough frequencies and the beam diverges so quickly it is difficult to route the THz with optics.
The Nelson group has developed the THz polaritonics platform to address these issues, where generation, amplification, control, and detection occur in a single compact chip.  Here, the chip is a 30 - 50 um thick slab of lithium niobate (LiNbO3) crystal. An intense optical pump pulse passes through the slab where it generates THz-frequency phonon-polariton wave via a nonlinear optical response in the crystal. The generated THz wave is guided down the slab, where it will interact with a machined air-gap, metallic microstructure, or sample deposited on the surface (see Figure 1 below).
Figure 1 Polaritonics geometry. The THz is generated by an ultrafast optical pump pulse and then guided down the crystal slab, where it can interact with a sample deposited on the surface.

THz Imaging

A key capability of the polaritonics chip is the ability to measure the full spatial profile of the electric field of the THz wave at each point in time as the wave propagates at the speed of light [Werley 2010].  This information can be played back as a video showing interactions of the wave with structures in or on the chip, providing exceptional insight into the behavior of photonic components.  This is possible because LiNbO3 is an electro-optic crystal, so the THz field induces a change in the index of refraction, which shifts the phase of the expanded optical probe beam used to detect the THz wave: 
We then use a phase sensitive imaging technique to record the induced shift, and step the time delay between pump and probe pulses to build up the full evolution of the wave.  See the movie theater for examples of movies collected using this technique.  (a) in the Figure 2 shows the optical setup for phase contrast imaging.  A phase mask in the Fourier plane of the lens introduces a 90 degree phase shift between the main beam and the diffracted light, which leads to interference and thus phase-to-amplitude conversion in the image plane.  (b) shows one frame from such a movie.  The light-gray rectangles are air gaps cut into the LiNbO3 slab.  On the left, part of the THz wave has reflected off the air gaps and on the right some has transmitted through the thin bridges between gaps.  Both reflected and transmitted waves are undergoing diffraction and interference.

Figure 2. THz imaging. (a) Phase contrast imaging. (b) An image of a THz wave reflecting off and transmitting through 5 slits, clearly demonstrating diffraction and interference.

THz Antennas

We recently used the polaritonics platform to study metal antennas deposited on the surface of the LiNbO3 slab [Werley 2012].  Pairs of half-wave antennas aligned end-to-end and separated by a small gap, like the one shown in (a) in the figure below, provide very large field enhancements in regions much smaller than the diffraction limit.  We studied these antennas for three purposes: 1. to develop a component for future high-speed devices that can interconvert propagating electromagnetic waves and subwavelength electronics, 2. to harness the antenna's field enhancement to generate very high amplitude electric fields for future nonlinear THz experiments, and 3. to improve fundamental understanding of antenna behavior for experiments at all frequency ranges.
Figure 3. A THz antenna. (a) Diagram of  a pair of half-wave antennas, showing field localization and enhancement at the antenna ends and in the small gap between them.  (b) An image of a resonant THz wave interacting with such an antenna deposited on the surface of the lithium niobate slab.  (c) A magnified view of (b) showing field localization and enhancement at the antenna ends and gap.
We used polaritonics imaging to map the THz field with λ/100 spatial resolution and fully understand the near-field profiled of the antenna [see (b) and (c) in Figure 3].  We directly measured E-field enhancements up to 40-fold and developed some simple models to predict field enhancement as a function of antenna length and gap size.  These insights are applicable at all frequency ranges and will aid the design of antennas for various applications including single-molecule fluorescence, surface enhanced Raman spectroscopy, near-field scanning optical microscopy.  In particular, our group want to use the extremely intense fields in the antenna gap to perform nonlinear THz spectroscopy.

THz Metamaterials

In 1967, Veselago postulated the existence of unnatural materials that have simultaneous negative permittivity, ε, and permeability, µ. These materials would have a negative refractive index (see Fig. 4). Only many decades later were these materials proven to exist by Smith and Pendry in a composite medium now termed metamaterials. In the same way that a material is made up of atoms that give rise to characteristic macroscopic properties, µ and ε, a metamaterial is made up of periodic microstructures or artificial atoms that give an effective response, µeff and εeff. Some interesting phenomena that result from such materials include negative refraction, superlensing, and cloaking.
Figure 4. Refraction with a negative index. (a) Refraction in a conventional positive index material with rays on opposite sides of the normal and the same sign of phase velocity. (b) Refraction in a negative index material with rays on the same side of the normal and negative phase velocity.
Electric and magnetic microstructures that are resonant at THz frequencies can be fabricated using lithography, where the dimensions and periodic spacings are smaller than the wavelength of light. Examples of these microstructures are shown in Fig. 5. Microstructures generally behave as damped harmonic oscillators, which leads to a negative response at frequencies near the resonant frequency w0.
Figure 5. Examples of electric and magnetic microstructures and the real part of the frequency-dependent permittivity and permeability function.
We are interested in learning more about the properties of negative index materials and how we can apply them to new systems and devices. With our capabilities in imaging fields, it may be possible to visualize negative refraction in a slab of LiNbO3, where a 2D array of metamaterials is lithographically deposited on the surface (see Fig. 6 for experimental geometry). Much like in the antenna study, using phase-contrast imaging [Werley 2010] we can temporally and spatially resolve the near- and far-field behavior of such materials.
Figure 6. Experimental geometry of a negative index slab waveguide, where an evanescent rightward propagating THz wave interacts with a 2D array of metamaterials.


Photonic Crystals

A photonic crystal is made of two or more materials that have different refractive indices arranged in a periodic fashion. Most commonly they are made by either cutting holes in a dielectric material or by placing rods of a dielectric in air. A cartoon is shown in Figure 7. Because of the periodicity of the material, photonic crystals exhibit optical properties not found in normal dielectrics. The most notable new characteristic is the presence of a photonic bandgap, i.e. a range of frequencies for which light cannot propagate inside of the crystal. If light incident on a crystal has a frequency that is in the bandgap it will be rejected with very high efficiency.

Figure 7. (a) A cartoon of a photonic crystal. The white circles are air holes which are cut into a piece of dielectric material. (b) Illustration of the photonic bandgap. In this case, the frequency of the red light is in the bandgap of the material and hence it is rejected while the green is transmitted through.

Photonic crystals can be used to build bends for redirecting light, splitters to divide light into different channels, and various kinds of filters. Previous work has focused on studying photonic crystals in the microwave regime for use in telecommunications. However, almost all this has focused on studying the light after it has propagated through the crystals, and it has been difficult to measure the fields directly within crystals themselves. Our work takes advantage of the imaging techniques that we have developed to study the fields within photonic crystals. These measurements can be compared with simulation and for time resolved studies by watching the fields as they propagate in the crystal. Using laser machining, we are able to fabricate THz-frequency photonic crystals by cutting air holes into thin lithium niobate slabs. We also work on developing new materials which can use electrical voltages and optical pulses to change the performance of the photonic crystals.

References

[Werley 2010] C. A. Werley, Q. Wu, K-H Lin, C. R. Tait, A. Dorn, and K. A. Nelson, Comparison of phase-sensitive imaging techniques for studying terahertz waves in structured LN, J. Opt. Soc. Am. B 27, 2350-2359 (2010).
[Werley 2012] C. A. Werley, K. Fan, A. C. Strikwerda, S. M. Teo, X. Zhang, R. D. Averitt, and K. A. Nelson, Time-resolved imaging of near-fields in THz antennas and direct quantitative measurement of field enhancement, Opt. Express 208551-8567 (2012).
[Ward 2006] D. W. Ward, E. R. Statz, and K. A. Nelson, Fabrication of polaritonic structures in LiNbO3 and LiTaO3 using femtosecond laser machining, Appl. Phys. A 86, 49-54 (2006).