Cerenkov Radiation in Photonic Crystals

Chiyan Luo, et al.

Science 299, 368 (2003);
DOI: 10.1126/science.1079549

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 REPORTS
the position, and t is the time. Bloch waves
Cerenkov Radiation in Photonic arise from the resonance of a planewave
source with the photon dispersion relation

Crystals ␻ n (k) ⫽ k 䡠 v (1)

where ␻ is the frequency, n is the band index,
Chiyan Luo, Mihai Ibanescu, Steven G. Johnson, the wave vector k can include an arbitrary
J. D. Joannopoulos* reciprocal lattice vector G, and ␻n(k) ⫽
␻n(k ⫹ G). The CR consists of modes satis-
In a conventional material, the coherent Cerenkov radiation due to a moving fying Eq. 1 (24 ), which can be found in k
charged particle is associated with a velocity threshold, a forward-pointing
radiation cone, and a forward direction of emission. We describe different
behavior for the Cerenkov radiation in a photonic crystal. In particular, this
radiation is intrinsically coupled with transition radiation and is observable
without any threshold. Within one particle-velocity range, we found a radiation
pattern with a backward-pointing radiation cone. In another velocity range,
backward-propagating Cerenkov radiation can be expected. Potential applica-
tions include velocity-sensitive particle detection and radiation generation at
selectable frequencies.

Downloaded from www.sciencemag.org on March 13, 2007

When a charged particle travels inside a medi- charge crosses a dielectric boundary or expe-
um, it can drive the medium to emit coherent riences an inhomogeneous dielectric environ-
electromagnetic energy called Cerenkov radia- ment, and the conventional CR, in which
tion (CR) (1). Extensively used in particle de- coherence is preserved throughout the medi-
tectors and counters (2), CR in a conventional um. Both effects are incorporated in our ap-
material possesses three key characteristics: it proach. However, unlike the Smith-Purcell
occurs only when the particle’s velocity ex- effect, in which radiation is generated via a
ceeds the medium’s phase velocity, the energy periodic grating but then propagates through
propagates only in the forward direction, and a uniform medium, this CR is generated and
there is a forward-pointing conical wavefront. propagates within the same crystal in the
These characteristics remain qualitatively un- form of Bloch waves. The properties of these
changed even in the presence of material dis- Bloch waves can be substantially different
persion (3–6). One possible source of unusual from waves in a uniform medium, leading to
CR is in a medium with simultaneously nega- effects not previously anticipated. In one
tive permittivity and permeability, commonly case, we can reverse the overall cone that
known as a negative-index material for its re- encloses all traveling electromagnetic energy.
versal of Snell’s law of refraction (7–12), in In another situation, we demonstrate a back-
which CR is predicted to flow backward; i.e., ward-propagating CR behavior reminiscent
opposite to the particle velocity (7). Another of that predicted in negative-index materials.
possibility exists near a periodic structure, These are very general results based on direct
where simple Bragg scattering of light can give solutions of Maxwell’s equations and should
rise to radiation without any velocity threshold. find applications in particle detection and
This was first confirmed by Smith and Purcell wave production techniques.
(13) in early experiments with electrons travel- For simplicity, we focus on a two-dimen-
ing near the surface of a metallic grating. CR sional photonic crystal (Fig. 1). Let a charge
has since been studied in one-dimensionally q move in the (01) direction of a square
periodic multilayer stacks (14, 15), and the lattice of air holes in a dielectric, in the xz
Smith-Purcell effect has been extended to near plane, with parameters as specified in the Fig. Fig. 1. Band structure and analysis of CR in a
the surface of dielectric structures (16, 17). A 1 legend. Figure 1A shows the calculated photonic crystal. (A) Transverse electric band
structure of a two-dimensional square lattice of
photonic crystal (18–20), where very complex transverse electric (the electric field in the xz air columns in a dielectric (dielectric constant ε
Bragg scattering is possible, presents a rich new plane, appropriate for CR) band structure of ⫽ 12) with column radii r ⫽ 0.4a, a being the
medium for unusual photon phenomena (21– this photonic crystal. We take the particle’s lattice period. The crystal structure and the
23). We reveal a variety of CR patterns that can motion to be in the z direction and consider a irreducible Brillouin zone are shown as insets. ⌫,
occur in a single photonic crystal under differ- path where the particle does not cross dielec- X, and M are, respectively, the center, edge
ent particle-velocity regimes. tric interfaces (Fig. 1B, inset). As a reference, center, and corner of the first Brillouin zone. (B)
Method of solving Eq. 1 in k space. CR occurs
CR in a photonic crystal arises from a the long-wavelength phase velocity (vc) of when the kz ⫽ ␻/v plane (dashed line) inter-
coherent excitation of its eigenmodes by the this photonic crystal is vc ⫽ 0.44c (where c is sects a photonic-crystal dispersion surface. Blue
moving charge. Its origin lies in both the the speed of light). The excited radiation can arrows indicate the group velocities of CR
transition radiation, which occurs when the be determined by treating the charge as a modes. (C) Method of obtaining CR cone
source with space-time dependence ␦(r–vt) ⫽ shapes. The group velocities for all modes ob-
兺k eik 䡠 r – ik 䡠 vt, that is, as a superposition of tained in (B) form a contour. ␣ is the cone angle
Department of Physics and Center for Materials Sci- for the mode with group velocity u, and ␣m
ence and Engineering, Massachusetts Institute of planewaves with different wave vectors k and gives the angle for the overall radiation cone
Technology, Cambridge, MA 02139, USA. frequencies k 䡠 v, where ␦ is the Dirac delta (gray dashed lines). The angular density of
*To whom correspondence should be addressed. E- function, e is the base of the natural loga- the arrows roughly reflects the CR angular
mail: [email protected] rithm, i is the unit of imaginary numbers, r is distribution.

368 17 JANUARY 2003 VOL 299 SCIENCE www.sciencemag.org

 REPORTS
space by intersecting the plane ␻ ⫽ k 䡠 v with charged particle in the same time. Thus, the possess a backward-pointing overall cone
the dispersion surface ␻ ⫽ ␻n(k) (Fig. 1B). radiation wavefront for each mode lies on a (␣m ⬎ ␲/2), according to the analysis of Fig.
The CR behavior in real space, however, “group cone” (3, 6 ) with its apex on the 1C. This is therefore the reversed-cone re-
must be obtained from the group velocity u ⫽ moving particle and a half-apex angle ␣, the gime. Such a reversed cone is forbidden by
⳵␻/⳵k; that is, the gradient vector to a disper- angle between v ⫺ u and v. A superposition causality (1) in a uniform passive medium.
sion surface, which can be shown to be the of all group cones gives the overall CR pat- 3) In the ⬃0.2c ⱕ v ⱕ ⬃0.4c regime, all
energy transport vector for each mode (25). tern, and the maximum angle ␣m of all such the radiation modes in the lowest emission
The emission angle is given by the direction ␣’s is the half-apex angle for the overall cone. band reside in the region ␲/a ⬍ kz ⬍ 2␲/a
of u. Moreover, the radiation pattern can be Propagating Bloch modes can only exist on with uz ⬍ 0, which implies that the energy
deduced from u via the group velocity con- the rear side of this overall cone, whereas the flows opposite to v in this band. The overall
tour (Fig. 1C). We plot both the charge ve- radiation fields are evanescent on the forward cone is now pointing forward and, as de-
locity v and the group velocities u of all the side, and across the overall cone the radiated scribed below, the radiation becomes colli-
CR modes in a velocity space (26 ). The field amplitude experiences a drop. In the mated in a backward direction. CR here is
magnitude of u is proportional to the distance special case of a uniform material, only the strongly similar to the predicted behavior in a
traveled by the wavefront of the associated G ⫽ 0 modes are excited and our approach negative-index material. However, because
photon mode, and the magnitude of v is pro- yields the characteristics of conventional CR. k⬘ 䡠 u ⬎ 0 in this regime (where k⬘ is the
portional to the distance traveled by the For an electron traveling near a grating sur- Bloch-reduced k in the first Brillouin zone),
face, one employs the dispersion relations of the photonic crystal may be regarded as an
air along with diffraction to obtain the Smith- effective positive-index medium (22). We

Downloaded from www.sciencemag.org on March 13, 2007

Purcell radiation. call this the backward-flux regime.
In the present photonic crystal, we solved 4) In the v ⱖ vc regime, the solution to Eq.
Eq. 1 using photon bands calculated by 1 starts from zero frequency, and the group-
planewave expansion (27). We focused on velocity contour becomes an open-ended
the solutions with the lowest frequencies; curve with positive uz. The charged particle
higher-order modes with larger G or in higher now travels faster than all of the excited
bands can be analyzed similarly. Figure 2 modes, and constructive interference is
shows the results for the CR emission fre- achieved throughout the whole photonic crys-
quency ␻, wave vector k, and group velocity tal. This behavior is identical to CR in a
u. We see that for v ⬍ ⬍ vc, the radiation normal dispersive medium. Hence, this is the
coalesces into Smith-Purcell resonances normal regime.
around ␻ ⬇ G 䡠 v. For larger v, the resonances The CR showed less interesting transition-
merge together to form emission bands out- al behavior for intermediate charge velocities
side which CR is inhibited (Fig. 2A). As v between these regimes. For example, when
increases, k and u within each emission band ⬃0.4c ⬍ v ⬍ ⬃vc, the CR showed a mixture
are strongly influenced by the photonic band of forward and backward emissions similar to
structure. We can identify four regimes of the that depicted in Fig. 1C.
charge velocity (Fig. 2, B and C) with four We confirmed our analysis by performing
qualitatively different CR behaviors in a pho- finite-difference time-domain (FDTD) simu-
tonic crystal: lations of radiation for a moving charge in
1) v ⱕ ⬃0.1c corresponds to the Smith- this photonic crystal (28). We reproduce in
Purcell regime, in which the CR arises pri- Fig. 3A the velocity diagrams from Fig. 2C
marily through constructive interference be- and present the resulting radiation-field sim-
tween consecutive unit cells and in the first ulations in Fig. 3B. To quantitatively demon-
emission band corresponds to the first res- strate the backward radiation, we also plot in
onance near kz ⫽ 2␲/a, where a is the Fig. 3C the simulated flux through a fixed
lattice period. The group velocity contour line perpendicular to v as a function of ␻. At
is approximately circular, with radius vc. the low velocity, v ⫽ 0.1c, the radiation
Because v ⬍ ⬍ vc, the overall wavefront shows a Smith-Purcell behavior of near-iso-
will be roughly circular and centered on the tropic wavefront. As the velocity increases to
slowly moving particle. v ⫽ 0.15c, the overall radiation cone indeed
2) The regime v ⬇ 0.15c is unique to the reversed as predicted. Further increasing of v
photonic crystal: The first and higher Smith- to v ⫽ 0.3c steers the radiation to the back-
Purcell resonances merge into one band, in ward direction, and if v is increased to v ⫽
which the slow photon modes near the pho- 0.6c ⬎ vc the familiar CR with a sharp for-
tonic band edge are in coexistence with the ward-pointing cone as in a uniform medium
fast modes. As can be seen from the group is recovered. The angular distribution of ra-
velocity contours, in going from v ⫽ 0.1c to diation is directly visible (Fig. 3B). When
Fig. 2. Calculated CR modes with the lowest v ⫽ 0.15c, the modes in the forward direction v ⫽ 0.1c or 0.15c, the radiation is distributed
frequencies for the photonic crystal of Fig. 1. begin to travel slower than the charged par- over a wide range of emission angles without
(A) The CR emission band structure (red region) ticle (and can even have negative group ve- producing a cone of intensity maxima. For
in the first photonic band as a function of v. locities), eventually producing a contour at v ⫽ 0.3c or 0.6c, however, the CR becomes
Colored vertical lines mark representative vs for
different CR behaviors. (B) The solution k for a
v ⫽ 0.15c that winds around without enclos- collimated, and a definite emission angle in
few vs indicated by the numbers in italics. (C) ing v. Because in this band there are some fast both the forward and the backward direction
The group velocity contours for the represen- modes in the forward direction whose uz ex- for most of the radiation energy can be ob-
tative values of v. ceeds v, the radiation pattern here should served. In particular, the crystal-induced dis-

www.sciencemag.org SCIENCE VOL 299 17 JANUARY 2003 369

 REPORTS
persion at v ⫽ 0.6c becomes so small that a these tails can exhibit a backward radiation centimeter, which should be amenable to di-
strong intensity peak cone is formed and effect as well. rect experimental observation.
almost overlaps with the overall cone. A clear The effects presented here can be extend- A number of applications also appear pos-
distinction between the CR behaviors for v ⬍ ed to three-dimensional photonic crystals sible. Particles traveling at speeds below the
vc and v ⬎ vc is that for v ⬎ vc the measured with little change. As a complete photonic phase-velocity threshold cannot be detected by
flux in the z direction is positive over the band gap in three dimensions is not required, conventional CR counters, and currently their
emission band, but for v ⬍ vc certain frequen- the crystal structure can be flexibly chosen. observation relies on other devices, such as
cy regions appear where the flux can be For experimental studies, an appropriate scintillation counters, proportional counters, or
negative (Fig. 3C). Because positive and neg- structure that quantitatively approximates our cloud chambers. These other devices, however,
ative flux values can occur at the same fre- calculations could be a square lattice of air lack the unique advantages of strong velocity
quency [e.g., at (␻a)/(2␲c) ⫽ 0.2], this pho- holes perforating a finite-height silicon slab, sensitivity and good radiation directionality
tonic crystal does not behave as a uniform interacting with fast electrons, and operated as in conventional CR (2). With a photonic
negative-index medium, as noted before. An- near the communication wavelength. The crystal, one should be able to achieve velocity
other distinction lies in the field pattern and is same physics should apply to dielectric-in- selectivity and distinctive radiation patterns
similar to that reported in (5) at a phonon air–type crystals as well. A practical issue is without any velocity threshold. Moreover, on
resonance frequency: The near-static, nonra- whether the radiation intensity is sufficiently the high-energy side, CR with a sharp radia-
diating field extends beyond the overall cone strong to be observable for small v. Our tion wavefront is possible for particles trav-
when v ⬍ vc, whereas for v ⬎ vc, the field numerical simulation indicates that, across a eling through an all-air path inside a photonic
outside the cone is strictly zero. These near- bandwidth of around 40%, the average radi- crystal, allowing complete absence of the

Downloaded from www.sciencemag.org on March 13, 2007

static fields create an artificial peak around ation energy is roughly in a ratio of 1:1.5:4: impurity scattering and random ionization
␻ ⫽ 0 in Fig. 3C for v ⬍ vc, (as in v ⫽ 0.1c) 20 for v/c ⫽ 0.1, 0.15, 0.3, and 0.6. Further- losses inherent in a dense medium. This
which we have verified to reduce to 0 for ␻ ⫽ more, the radiation intensity at small v may should improve the performance of present
0 with increasing computational cell sizes even be much larger than these numbers in detectors. Finally, the CR frequency is set by
and time steps. Finally, there are high- narrow bandwidths around specific frequen- the photonic crystal and is thus selectively
frequency radiation “tails,” corresponding to cies, because of the unusual photon density of scalable beyond optical wavelengths, open-
higher-order radiation, behind the charge in states in a photonic crystal. In conventional ing up the possibility of flexible radiation
all cases of Fig. 3B. The higher order modes CR, for v ⬎ vc an electron can emit hundreds sources for frequencies that are otherwise
typically have smaller group velocities and of photons per centimeter of its path. Thus, difficult to access.
thus form dense forward-pointing cones of for the velocities studied here, the emission
smaller angles, as first predicted in (6 ) (for rates correspond to a range starting from References and Notes
1. L. D. Landau, E. M. Liftshitz, L. P. Pitaevskii, Electro-
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Fig. 3. FDTD simulation results for CR in the photonic crystal of Fig. 1. Each column represents the Phys. Rev. B 65, 201104 (R) (2002).
23. C. Luo, S. G. Johnson, J. D. Joannopoulos, Appl. Phys.
results for the value of v shown on the top. (A) Overall radiation cone shapes (dashed lines) Lett. 81, 2352 (2002).
deduced from the group velocity contours in Fig. 2C. (B) Distribution of the radiated magnetic field 24. The CR modes are excited with a strength propor-
Hy. Blue, white, and red represent negative, zero, and positive field values, respectively. The color tional to the density of radiation states and qv 䡠
tables are chosen separately for best illustration in each case. (C) The frequency spectrum of the e*k⬘nG, where k⬘ is the Bloch-reduced k in the first
electromagnetic flux along z through a line perpendicular to v, in arbitrary units (a.u.). Brillouin zone; G ⫽ k – k⬘; and e*k⬘nG is the G-Fourier

370 17 JANUARY 2003 VOL 299 SCIENCE www.sciencemag.org

 REPORTS
component of the Bloch electric field, as in Ekn ⫽ 兺G 28. The simulation uses a thick perfectly matched layer 30. M. Koshiba, Y. Tsuji, S. Sasaki, IEEE Microwave Wireless
eknGei(k ⫹ G) 䡠 r. boundary region that overlaps 10 periods of the Components Lett. 11, 152 (2001).
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in (29), though it now represents group velocities of tion and whose position depends on time. Research Initiative program (grant no. N00014-01-1-
different frequencies. 29. M. Born, E. Wolf, Principles of Optics: Electromagnetic 0803).
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(2001). Light (Cambridge Univ. Press, New York, ed. 7, 1999). 18 October 2002; accepted 5 December 2002

A Reversibly Switching Surface chain alkanethiolate monolayers on gold

within the range of chemical stability of the
SAM (18). In other words, conventional
Joerg Lahann,1 Samir Mitragotri,2 Thanh-Nga Tran,1 SAMs are too dense to allow conformational
Hiroki Kaido,1 Jagannathan Sundaram,2 Insung S. Choi,1* transitions and consequently do not allow for
Saskia Hoffer,3 Gabor A. Somorjai,3 Robert Langer1† switching. To explore SAMs as a model sys-
tem for switching, we must establish suffi-
We report the design of surfaces that exhibit dynamic changes in interfacial cient spatial freedom for each molecule. Once
properties, such as wettability, in response to an electrical potential. The change a low-density SAM is created, preferential

Downloaded from www.sciencemag.org on March 13, 2007

in wetting behavior was caused by surface-confined, single-layered molecules exposure of either hydrophilic or hydropho-
undergoing conformational transitions between a hydrophilic and a moderately bic moieties of the SAM to the surrounding
hydrophobic state. Reversible conformational transitions were confirmed at a medium could be exploited for the switching
molecular level with the use of sum-frequency generation spectroscopy and at of macroscopic surface properties.
a macroscopic level with the use of contact angle measurements. This type of (16-Mercapto)hexadecanoic acid (MHA)
surface design enables amplification of molecular-level conformational tran- was chosen as a model molecule because it (i)
sitions to macroscopic changes in surface properties without altering the chem- self-assembles on Au(111) into a monolayer
ical identity of the surface. Such reversibly switching surfaces may open pre- and (ii) has a hydrophobic chain capped by a
viously unknown opportunities in interfacial engineering. hydrophilic carboxylate group, thus poten-
tially facilitating changes in the overall sur-
Interfacial properties, such as wetting behav- using an active stimulus, such as an electrical face properties. To create a monolayer with
ior, are defined by the molecular-level struc- potential, to trigger specific conformational sufficient spacing between the individual
ture of the surface (1). Diverse modification transitions (e.g., switching from an all-trans MHA molecules, we used a strategy that
procedures have been used to permanently to a partially gauche oriented conformation; exploits synthesis and self-assembly of a
alter wettability (2– 4 ). Control of wettability see Fig. 1). Amplification of conformational MHA derivative with a globular end group,
has been recently demonstrated by elegant transitions to macroscopically measurable which results in a SAM that is densely
methods including light-induced (5–6 ) and changes requires synergistic molecular reori- packed with respect to the space-filling end
electrochemical surface modifications entations of ordered molecules. In principle, groups but shows low-density packing with
(7–10). These systems require chemical reac- this is attainable with a single-molecular lay- respect to the hydrophobic chains. Subse-
tions in order to control wettability. er, such as a self-assembled monolayer quent cleavage of the space-filling end
We demonstrate an alternative approach (SAM) of alkanethiolates on gold (15). How- groups establishes a low-density SAM of
for dynamically controlling interfacial prop- ever, the dense molecular packing in SAMs MHA. The spatial dimensions of the precur-
erties that uses conformational transitions and the strong interactions between the meth- sor molecule to be used were adapted to
(switching) of surface-confined molecules. ylene groups restrict dynamic molecular mo- match the optimum alkanethiolate density for
Polymers have been shown to undergo con- tions to the outermost atoms (16, 17). All in conformational rearrangements.
formational reorientations when changed situ evidence so far indicates that applied The equilibrium low-energy conformational
from one solvent to another (11) or from one electrical potentials have no effect on long- state of each of the sparsely packed MHA
temperature to another (12, 13) because of
phase transitions between a well solvated and
a poorly solvated state (14 ). In contrast, our
approach maintains the system’s environment
unaltered (including solvent, electrolyte con-
tent, pH, temperature, and pressure) while

1
Department of Chemical Engineering, Massachusetts
Institute of Technology (MIT ), 45 Carleton Street,
Cambridge, MA 02139, USA. 2Department of Chemi-
cal Engineering, University of California at Santa Bar-
bara, Santa Barbara, CA 93106, USA. 3Department of
Chemistry, University of California at Berkeley, Ma-
terial Science Division, Lawrence Berkeley Laboratory,
Berkeley, CA 94720, USA.
*Present address: Department of Chemistry and
School of Molecular Science (BK21), Korean Advanced
Institute of Science and Technology, Daejeon 305- Fig. 1. Idealized representation of the transition between straight (hydrophilic) and bent (hydro-
701, Korea. phobic) molecular conformations (ions and solvent molecules are not shown). The precursor
†To whom correspondence should be addressed. E- molecule MHAE, characterized by a bulky end group and a thiol head group, was synthesized from
mail: [email protected] MHA by introducing the (2-chlorophenyl)diphenylmethyl ester group.

www.sciencemag.org SCIENCE VOL 299 17 JANUARY 2003 371