United States
 Environmental Protection
 Agency
 Health Effects
 Research Laboratory
 Research Triangle Park NC 27711
 Research and Development
 EPA/600/S1-87/002 Aug. 1987
 Project Summary
 Millimeter-Wave Emissivity of
 Cellular  Systems
 K. H. Illinger
  A general analysis is presented of the
millimeter-wave and far-infrared spec-
troscopic properties of in vivo cellular
systems, and of the boson  radiative
equilibrium with steady-state nonequili-
brium molecular systems. The frequency
threshhold of spectroscopic properties
associated with such nonequilibrium ef-
fects is (roughly) estimated to be as low
as ~100 GHz, if the Frbhlich vibrational
model can  be  invoked  for  cellular-
membrane systems. On this basis, the
rationale for the specific experimental
protocol employed was further to utilize
the fact that in a photosynthetic  pre-
paration the onset  and disappearance
of  the  nonequilibrium  state  can  be
switched by modulating the  optical-
illumination input. The negative findings
of  the  present  V-band (50-75 GHz)
radiometric study on in vivo  chloralla
pyrenoidosa algal cells appear to con-
firm the absence  of non-Planckian
emissivity features  in the total radio-
metric  study  on  saccharomyces
cerevislae near 42  GHz (3), but does
not negate totally the existence of non-
equilibrium  emissivity terms in  the
frequency range studied. Limitations of
radiometer  sensitivity, in spite of the
S/N enhancement achieved through the
AM-modulation  technique,   and/or
damping of the non-Planckian emissivity
features may have vitiated their detec-
tion. More fundamentally, the frequency
threshhold  for such  properties may
indeed lie at higher  frequencies, in the
far-infrared region. An order of magni-
tude of  refinement in the  theoretical
models will be required to serve as a
reliable guide for the prediction of such
frequency threshholds.
  This Project Summary was developed
by EPA's Health Effects Research Labo-
 ratory, Research Triangle Park, NC, to
 announce key findings of the research
 project that Is fully documented In a
 separate  report of the same title (see
 Protect Report ordering Information at
 back).

 Discussion
  As a consequence of the existence of
 nonequilibrium thermodynamic subsys-
 tems in in vivo biological entities, in-
 cluding cellular  systems, spectroscopic
 features may be expected to arise which
 differ from those exhibited by ordinary
 equilibrium thermodynamic systems. A
 detailed theoretical analysis identifies, in
 particular, the emissivity function  as a
 targetable observable in this category.
 The emissivity function, t(w),  is defined
 as the  ratio of the aetuat emission in-
 tensity of the system under consideration,
 at a given frequency, to that of an ideal
 blackbody at the same temperature. The
 emission  intensity is the photon energy
 emitted across a  unit  surface area, per
 unit  time,  into a solid  angle  of 2?r
 steradians, and is proportional to the
 value of the generalized distribution func-
 tion of photons over frequencies, n(o>), at
 the given  frequency, characteristic of the
 thermodynamic system under considera-
 tion. If the system is an ideal blackbody,
 n(oj) is  the Planck function and e(cu)  is
 unity and  frequency-independent.
  A general thermodynamic  analysis
 shows  that nonequilibrium  systems
 should exhibit frequency-dependent fea-
 tures in t(tu). If the Froehlich vibrational
 model is applied to cellular systems and
the cellular membrane is identified as
the  locus of  nonequilibrium  thermo-
dynamic processes, a frequency regime
as low as ~ 100 GHz is credible for the
possible existence of non-Planckian fea-

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tures. This study utilized in vivo photo-
synthetic algal cells [chlorellapyrenoidosa
(American Type Culture Collection, in the
form of their strains ATCC 22521, 7516
and 11469)] as the experimental model
system,  since  the photosynthetic  ap-
paratus is located in the cell membrane,
and since photosynthetic processes lend
themselves directly to external modula-
tion. In consequence, the temporal onset
and disappearance of these nonequili-
brium processes are externally control-
lable, and the opportunity is provided to
improve the S/N ratio of measurements
of the contribution of the nonequilibrium
subsystem(s) to the total emissivity func-
tion, the preponderant portion of which
arises  from  the Planckian  background
from the remainder of the system.
   Millimeter-wave  radiometry  systems
usually operate within the frequency
regions encompassed  by  individual
wavequide systems. This study employed
V-band  [WR-15], 50-75 GHz, to roughly
approximate the  frequency  domain
charted in the application of the Froehlich
model to the photosynthetic chloroplast.
The latter consists of  a flat, double-
membraned configuration, with a  mem-
brane thickness between 100-200 A, the
site of the photosynthetic apparatus and
the putative  locus of longitudinal vibra-
tions invoked in the  model. A serious
caveat in any generalization that  might
be made from the  results of this type of
study arises from the combination of the
crudeness of the frequency-range esti-
mate from theory and the inherent nar-
row-bandedness  of microwave and
millimeter-wave waveguide systems.
   The emissivity of the cellular prepa-
ration was measured using a 50-75 GHz
radiometer,  with  its detection circuit
phase-locked to the optical  illumination
of the sample in the  wavelength  range
centered  at 4900 A (±350 A), AM-
modulated by a precision optical chopper
at 100 Hz, to accomodate the response
time constant of the photosynthetic  ap-
paratus of the preparation, and to provide
selectivity and S/N ratio enhancement of
the radiometer signal arising from pro-
cesses associated with the photosynthetic
apparatus. The  source of  the optical
illumination was a 1000W Xe lamp, fol-
lowed  by standard components of an
optical  train, including a (distilled-H20)
broadband infrared filter and optical filters
selected to tailor the illumination to the
wavelength response function of the
cellular  preparation.  Millimeter-wave
emission from the sample was measured
at an angle of 90° to the optical-illumina-
tion axis, with the  cell preparation con-
tained in a quartz cuvette, transparent to
both visible light and  millimeter-wave
emission. In the context of the present
experiments, the task of the radiometer
was to detect any response, phase-locked
to the  optical illumination, within a
primary-illumination ra nge of 200-1OOOW
total (regulated and calibrated) power, of
the cell preparation.
  The local-oscillator (LO) arm  of  the
radiometer  originated in  a set of three
klystron oscillators spanning the 50-75
GHz range, and was coupled to the sample
arm and the detection-system arm via
broadband (50-75 GHz) ferrite  isolators.
The frequency axis  of the  radiometer
signal was provided by measurement of
the LO  frequency by means of a mil-
limeter-wave electronic counter and sub-
sequent conversion of  its frequency
output via  a  digital/analog  (D/A) con-
verter to a voltage analog signal to com-
prise the Y-axis of an X/Y recorder output.
Under typical  experimental  conditions,
frequency resolution thus obtained is
equal to or better than 0.1 MHz, over the
entire V-band frequency  range, and
frequency tracking of the LO is automatic.
A separate power-measurement loop
permits determination of the LO relative
power across a given klystron mode, as a
function of LO frequency. The primary
element of the  radiometer detection
system  is  a  broadband  (50-75 GHz)
harmonic  mixer matched to an  inter-
mediate-frequency (IF) amplifier, the latter
rejecting IF  signals below ~ 500 MHz
and above ~ 1500 MHz. Electronic tuning
of  the  LO,  by  means of  its reflector
voltage, moves the center of this IF detec-
tion window (bandwidth  ~  1000 MHz)
across the klystron mode. Director moni-
toring of radiometer  performance is ac-
complished by feeding the output of the
IF  amplifier directly into a (0-2  GHz)
spectrum  analyzer.   Radiometry of the
sample  preparation  is  achieved  by
entering the output  of the  IF amplifier
into a microwave video  detector, thus,
converting that output into a dc voltage.
The phase-lock synchronization  loop,
externally synchronized to the precision
optical chopper,  is engaged via a phase-
sensitive lock-in amplifier which accepts
the dc radiometer-output signal. Finally,
the radiometer-signal axis, from the out-
put of the lock-in amplifier, is combined
with the frequency  axis,  from the elec-
tronic counter and  D/A converter, to
present the radiometry data on an X/Y
recorder.
  The present study  failed to detect any
(non-artifactual) frequency-dependent
features m the radiometry signal phase-
locked to the optical illumination of th«
photosynthetic algal-cell preparation
Among the possible explanations for sucf
a finding, two are salient. The centra
modality of  the radiometer experimen
(direct AM-modulation of the  photosyn
thetic process) may have been vitiated b>
insufficiently favorable S/N ratio char
acteristics of any non-Planckian features
in the emissivity. This would render the
sensitivity  of the current radiometei
design incapable of detecting  such fea-
tures, in a manner which excludes arti-
facts of millimeter-wave waveguide
circuits. From a mechanistic standpoint,
any of three (heuristic) parameters ma\
have contributed to such a possibility, (a
the  low concentration  of subsystems
which undergo nonequilibrium processes,
per unit volume, compared to the (bulk;
system near equilibrium; (b) low absolute
emission intensity associated with any
non-Planckian features;  and/or (c)
damping of any non-Planckian  emissivity
features, with an attendant reduction in
S/N ratio,  within  a given frequency
interval.
  The second case arises from the central
question, to which existing theory is only
a very rough guide, concerning the low-
frequency  threshhold,  w,,   of  non-
Planckian  features.  If (n  01,/«T) -4 1 is
inadmissible as an assumption for cellular
systems, no non-Planckian features are
expected in the frequency range studied,
with Ts300°K, and their absence in the
present study is not inconsistent with the
thermodynamic or the generalized Froeh-
lich model, but would imply that definitive
refinement in the theory  is required for
the prediction of their (frequency) range
of existence.

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     K. H. Illinger is with Tufts University. Medford, MA 02155.
     Jamas R. Rabinowitz is the EPA Project Officer (see below).
     The complete report, entitled "Millimeter- Wave Emissivity of Cellular Systems,"
      (Order No. PB 87-175 840; Cost: $ 11.95, subject to change) will be available
      only from:
            National Technical Information Service
            5285 Port Royal Road
            Springfield, VA 22161
            Telephone: 703-487-4650
     The EPA Project Officer can be contacted at:
            Health Effects Research Laboratory
            U.S. Environmental Protection Agency
            Research Triangle Park, NC 27711
United States
Environmental Protection
Agency
Center for Environmental Research
Information
Cincinnati OH 45268
                                                                                                ;  : 0 2 1.:
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