Optimized continuum x-ray emission from

laser-generated plasma
Cite as: Appl. Phys. Lett. 117, 251106 (2020); https://doi.org/10.1063/5.0033629
Submitted: 17 October 2020 • Accepted: 05 December 2020 • Published Online: 22 December 2020

A. Krygier, G. E. Kemp, F. Coppari, et al.

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 Applied Physics Letters ARTICLE scitation.org/journal/apl

Optimized continuum x-ray emission from

laser-generated plasma
Cite as: Appl. Phys. Lett. 117, 251106 (2020); doi: 10.1063/5.0033629
Submitted: 17 October 2020 . Accepted: 5 December 2020 .
Published Online: 22 December 2020

A. Krygier,1,a) G. E. Kemp,1 F. Coppari,1 D. B. Thorn,1 D. Bradley,1 A. Do,1 J. H. Eggert,1 W. Hsing,1

1 2 1 1 1
S. F. Khan, C. Krauland, O. L. Landen, M. J. MacDonald, J. M. McNaney, H.-S. Park,1 B. A. Remington,1
3 1 1 1
M. Rubery, M. B. Schneider, H. Sio, and Y. Ping

AFFILIATIONS
1
Lawrence Livermore National Laboratory, 7000 East Ave, Livermore, California 94550, USA
2
General Atomics, San Diego, California 92121, USA
3
Atomic Weapons Establishment, Aldermaston, Reading, Berkshire RG7 4PR, United Kingdom

a)
Author to whom correspondence should be addressed: krygier1@llnl.gov

ABSTRACT
We study continuum x-ray emission from hot plasma at the National Ignition Facility (NIF). We find that the x-ray yield in the multi-keV
photon energy range is larger in Ti than in Ag or Au. This apparent paradox is due to Ti K-shell vacancies generated by the extraordinary
energy density achieved by the NIF lasers. This is supported by direct observations of large continuum enhancement above the Ti K-series
limit due to both free–bound (recombination) emission and strong Lya (H-like) emission. Detailed calculations agree well with our measure-
ments and support our conclusions.
C 2020 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://
V
creativecommons.org/licenses/by/4.0/). https://doi.org/10.1063/5.0033629

X-ray emission from matter pervades the universe and plays an
important role in the high-energy density (HED) regime (105 J/cm3).
For example, the emission and absorption of x-rays controls the ther-
mal state and evolution of stellar interiors.1 Properties of solar flares
are determined by analyzing keV x-ray emission.2 In addition, studies
of x-ray-matter interactions in extreme environments, such as radia-
tion hardness studies,3,4 radiation-dominated astrophysical phenom-
ena,5–7 and inertial confinement fusion,8 use multi-keV x-ray sources.
Inertial confinement fusion implosions are also a strong source of
keV-range continuum x-ray emission.9
Nanosecond pulses of keV-range continuum x-rays have gener-
ated significant interest as a backlighter probe10–17 for high-pressure
materials science experiments. Among many applications, material
strength experiments18–20 use nanosecond pulses of 10–100 keV
x-rays for in situ sample radiography. EXAFS21–23 and single crystal
phase and strain anisotropy measurements24,25 use nanosecond broad-
band multi-keV x-ray pulses. In general, increased x-ray flux in the
given range improves data quality.
The National Ignition Facility’s (NIF) high-power lasers can be
used to heat samples to multi-keV temperatures, generating nanosec-
ond, multi-keV x-ray pulses. Inverse bremsstrahlung (IB) dominates
laser absorption in this regime as electrons gain energy through
collisions while oscillating in the laser field. The IB inverse absorption
length scales as / Z 2 ne ni Te3=2 ln ðKei Þ,26 where Z  is the ionization
state, ne is the electron density, ni is the ion density, Te is the electron
temperature, and ln ðKei Þ is the Coulomb logarithm. However, light
cannot propagate in plasma when ne > nc  1:1  1021 cm3 =k2lm ,
where klm is the laser wavelength in lm. At the NIF, klm ¼ 0:351 lm
and nc ¼ 8.9 1021 cm3. Since ni ¼ ne =Z  in charge neutral plasma,
IB scaling in realistic laser plasma varies as / Z  n2e Te3=2 ln ðKei Þ. This
suggests that the volume adjacent to the critical surface (ne ¼ nc con-
tour) dominates laser absorption. Pre-heating solid-density samples
with a picketed pulse increases this volume and can increase the
keV-range x-ray yield in laser-heated plasma.27 Low density foam
and gas-pipe targets are another approach concurrently under
development.14,16,17
The two dominant modes of keV-range continuum emission in
HED plasma are free–free (bremsstrahlung) and free–bound (recom-
bination) x-ray emissions. Free–free emission scales as / Z 2 ne ni Te1=2
/ Z  n2e Te1=2 , following the above laser-plasma arguments. This natu-
rally suggests that the increasing atomic number (Z) should increase
continuum emission. Free–bound emission occurs by recombination
of plasma electrons into open bound states; the emitted photon’s
energy is the sum of the kinetic and bound state binding energies,

Appl. Phys. Lett. 117, 251106 (2020); doi: 10.1063/5.0033629 117, 251106-1
C Author(s) 2020
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 Applied Physics Letters
producing continuum emission in plasma. The ratio of free–bound to
free–free radiation for recombination into shell n is nn =n3 En =
Te eðEn =Te Þ ,28 where nn is the number of holes in shell n and En is the
shell’s single-electron ionization energy (H-like in the K-shell, etc.).
Free–bound emissions can become very strong as Te becomes large
enough to create vacancies in shell n (Te  En); however, the 1/Te
factors limit free–bound yield at high Te creating optimal conditions
for Te  En. The multi-keV Te possible with NIF lasers ionizes up to
period 4 transition metal K-shells, motivating their use for multi-keV
continuum generation.
Here, we report results from NIF experiments investigating x-ray
emission from Ti, Ag, and Au foils (Z ¼ 22; 47; 79, respectively).
Figure 1 shows our experimental configuration. A total of 72 NIF
lasers (44 on front and 28 on back) heat foil samples over several
experiments (see Table I). The main pulse shape is a 2-ns quasi-square
with a peak power of 150 TW and a peak irradiance of 4.4  1015
W/cm2 (Fig. 1 inset); all but the Au shot also have a lower power
picket (peak 35 TW, 1  1015 W/cm2).
Figure 2 shows time-integrated 6–25 keV x-ray spectra recorded
using an NIF Survey Spectrometer29 (NSS, see the supplementary
material). In Au samples, the picketed pulse shape increases spectral
intensity by 4X over Au across the NSS energy range. Ag samples
produce similar continuum spectral intensity over this range. Below
21 keV, both experiments using Ti samples yield higher spectral
intensity than Ag or Au by up to 4X. Based on the continuum emis-
sion slope, Au and Au are the hottest, followed by Ag, with Ti being
the coolest. The repeated Ti experiment yields nearly identical spectra
suggesting high repeatability.
Figure 3(a) shows time-integrated Ti x-ray emission spectral
intensity recorded by Virgil30,31 (see the supplementary material).
X-ray spectra predicted by the radiation hydrodynamics code HYDRA32
(see the supplementary material) run in one-dimensional geometry
overlay the experimental data. We find good agreement with the
continuum and many bound–bound features. Under these conditions,
the large number of atomic energy levels necessitates the use of
super-configurations33 that lead to discrepancies seen in some emis-
sion energies [Fig. 3(a)]. We find that plasma conditions around
ne ’ 3  1021 cm3 and Te ’ 3:2 keV dominate keV-range radiation
FIG. 1. The experimental setup. Instruments recording x-ray spectra, x-ray emis-
sion images, and temporal x-ray emission are indicated by the target chamber
polar-azimuthal angle. The inset shows pulse shapes with (N190430-2) and without
(N181010-3) pickets. The non-picketed pulse shape is translated to overlap the
peak power plateau.
Appl. Phys. Lett. 117, 251106 (2020); doi: 10.1063/5.0033629
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TABLE I. Summary of discussed NIF experiments. Shots are identified by their
sample throughout; the asterisk denotes a non-picketed pulse shape. dz is the sam-
ple thickness; EP and EL are the picket and main pulse energies, respectively.
Shot Sample dz (lm) EP (kJ) EL (kJ)
N181010-3 Au 
2 0 266.1
N190115-1 Au 2 28.2 316.6
N190430-2 Ag 4 28.3 304.3
N190130-2 Ti 7 28.5 310.0
N190925-1 Ti 7 28.5 312.8
emission in Ti and correspond to Z ¼ 20.7. Moreover, the strong Lya
feature at 4.96 keV in the Virgil and HYDRA spectra arises from
hydrogen-like states, confirming the K-shell vacancies predicted by
21
HYDRA. In similar HYDRA simulations of Ag, we find ne ’ 2:1  10
cm3, Te ’ 6:4 keV, and Z  ¼ 40:3, consistent with the assertion of
hotter Ag plasma from the NSS data and a slightly vacant L-shell.
We investigate the continuum x-ray emission processes with the
hybrid-structure atomic kinetics code SCRAM.34,35 Figure 3(b) shows
SCRAM simulation results for free–free and free–bound x-ray emission
contributions for Ti and Ag in experimentally representative condi-
tions (ne ¼ 3  1021 cm3 and Te ¼ 4 keV). As expected, Ag yields
stronger free–free emission than Ti; however, this is a fraction of
the total continuum. Above the Ti K-series limit (6.1 keV), Ti
free–bound emission is 7–10 times larger than free–free, similar to the
jump observed in the measured and predicted x-ray spectra in (a). The
theoretical scaling for Ti using Z  ¼ 20.9 from the SCRAM simulations
and the hydrogen-like En ¼ 6:626 keV gives 7.9, in agreement with
SCRAM. The free–bound enhancement in Ag predicted by SCRAM is only
2.2, similar to the ratio of 2.9 given by the analytic expression, and the
continuum total is lower than that for Ti.
Figure 3(c) shows the ratio of free–bound to free–free x-ray emis-
sion calculated by SCRAM at 18 keV (above the K-series limit across
scanned materials) vs Z for ne ¼ 3  1021 cm3 and Te ¼ 4 keV com-
pared with the analytical expressions for the K- and L-shells (using Z 
from the corresponding SCRAM calculation). Atoms lighter than Ti
(Z < 22) have less than one bound electron, and the increase in En
FIG. 2. Raw x-ray emission spectra for laser-driven planar foils at the NIF are plot-
ted; Au (blue and purple curves), Ag (orange curve), and Ti (green and red curves)
foils were studied. The small discontinuity at 13.4 keV in the curves is due to
increased absorption above the Br K edge, an image plate (IP) active layer compo-
nent. The broad peaks at 22.5 keV (orange curve) and 9–12 keV (blue and
purple curves) correspond to the Ag Hea complex and Au L-series, respectively.
117, 251106-2
 Applied Physics Letters
FIG. 3. Time-integrated experimental x-ray spectral intensity (green curve) recorded
by Virgil and predictions from HYDRA (black curve) are shown in (a). In (b), SCRAM x-
ray emission simulations show free–free (F–F, dashed curves) and free–bound
(F–B, solid curves) emission contributions in Ag and Ti. The jump in x-ray emission
from free–bound transitions at 6.1 keV corresponds to the Ti K-series limit; the
jumps in Ag free–bound x-ray emissions at 2.5 keV and 5.8 keV correspond to
the M- and L-series limits, respectively. Panel (c) shows SCRAM predictions for the
free–bound to free–free emission ratio at 18 keV vs Z (black circles); the number of
bound electrons (Z  Z  ) is in blue. The shaded regions highlight the boundaries
for 1, 2, and 3 bound electrons; the ratio starts to decrease as Z  Z  becomes
>1. The analytical expression for K-shell (dashed brown curve), L-shell (dotted
brown curve), and combined (solid brown curve) free–bound emission is also
shown. All SCRAM calculations use ne ¼ 3  1021 cm3 and Te ¼ 4 keV.
with Z increases the free–bound yield. The inner shell of atoms heavier
than Ti have higher occupancy, and the free–bound contribution
decays due to diminished hole quantity. The disagreement between
the analytical and the SCRAM calculations near Z  Z  ¼ 2 is due to
the average Z  not adequately describing the distribution of ionization
states close to the filling of the K-shell.
Figure 4 shows temporally resolved x-ray emission in the photon
energy ranges of 1.2–7.2 keV and 7–20 keV using Dante36 and
SPIDER,37 respectively. Dante uses filtered fast x-ray diodes, and
SPIDER uses a filtered streak camera. Each configuration yields differ-
ent emission patterns to help understand the spectral results. The
emission recorded by both instruments persists until the laser turns off
on every experiment, ruling out sample burn through limiting the
overall x-ray yield. Additionally, the two Ti shots show nearly identical
SPIDER emission history, further indicating high repeatability.
Emission recorded by SPIDER from the non-picket laser pulse
for Au initially rises with the quasi-square laser pulse (sharper than
Appl. Phys. Lett. 117, 251106 (2020); doi: 10.1063/5.0033629
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FIG. 4. Panel (a) shows integrated 7–20 keV x-ray emission vs time recorded by
SPIDER (11.5 lm Zr filter) for Ti, Ag, Au, and Au. The inset shows SPIDER sensi-
tivity to a 4 keV exponential distribution. Panels (b)–(e) show 1.2 (navy curves), 3.0
(royal blue curves), and 7.2 keV (light blue curves) Dante channels from Au, Au,
Ag, and Ti shots. Laser pulses are shown by dashed pink curves. The Au data are
translated to overlap the laser pulse plateaus; each Dante trace is normalized.
the pulse with a picket, see the inset of Fig. 1), increases in magnitude
throughout its duration, and rapidly ceases with the end of the laser
pulse. The Dante data show a similar trend, with lower x-ray energies
(navy curves) rising earlier than higher energies (light blue curves),
indicating a combination of increasing emitting volume and heating
with time, as the laser remains on. The 2 ns pulse heats and expands
the sample, increasing the radiation losses and the emitting volume.
Comparing SPIDER sensitivity [inset of Fig. 4(a)] and NSS spectra, the
SPIDER data for Au (and Au) are dominated by L-shell emission.
While the L-shell is not expected to be ionized in these conditions,38
the overall yield should nevertheless increase as the emitting volume
increases. The rapid decay of keV x-ray emission with the end of the
laser pulse is characteristic of systems in this regime.
The Au (picket drive) SPIDER signal closely mimics the laser
pulse shape: emission rises over the first 0.6 ns (similar to the laser
pulse), plateaus in the center, and quickly decays when the laser turns
off. The Dante data show similar results, with all channels rising
quickly, plateauing, and then falling quickly when the laser turns off.
Whereas the Au Dante data suggest heating- and emitting-volume
expansion throughout the main drive, the Au Dante data suggest rapid
heating. The Au and Au x-ray spectra in Fig. 2 show the same slope
(ignoring bound–bound transitions), suggesting that Te is the same.
Combined with no SPIDER signal between the picket and main pulses
(1.5–4.5 ns in Fig. 4), this indicates that the picket primarily increases
the emitting volume by pre-expansion.
Like Au (picket drive), emission from Ag increases rapidly with
the main pulse. However, unlike Au, the emission increases through-
out the main pulse before rapidly decaying as the laser turns off. The
3.0 keV channel of Dante is sensitive to Ag L-series emission and
117, 251106-3
 Applied Physics Letters
correspondingly rises slightly faster than the other two channels that
are more sensitive to the continuum; fluctuations in the 7.2 keV data
are due to noise. The overall bound–bound emission is less efficient
than in Au, due to having fewer electrons and comparatively lower
binding energies. In our simulations, the end of the rapid increase in
emission roughly corresponds to Ag becoming oxygen-like, indicating
the onset of significant L-shell ionization and resulting in enhanced
free–bound radiation.
Finally, the Ti SPIDER signal rises more slowly, reaching near-
peak emission 1.3 ns after the main pulse’s leading edge. This is
likely due to weak bound–bound transitions and/or lower IB absorp-
tion due to the low Z. The Dante data confirm this as the channels rise
in order of increasing energy, indicating heating throughout the drive.
The Virgil spectra show that the Ti K-series limit increases to
6.1 keV (from 4.966 keV), consistent with our HYDRA simulations.
The high ionization state inferred from the HYDRA/SCRAM calculations
simultaneously depletes L- and M-shell bound–bound transitions and
increases free–bound contributions. As with Ag, the temporal emis-
sion history from Ti is bimodal. Unlike Ag, the rate of change of Ti
x-ray emission increases just after the laser pulse’s leading edge
(5.15 ns). This may correspond to the onset of strong free–bound
emission as the K-shell becomes ionized. In our simulations, this
change approximately corresponds to the onset of He-like states in Ti;
the average atomic configuration contains a distribution of ionization
states that include many H-like atoms. This is especially likely as
SPIDER is sensitive to energies associated with Ti K-shell free–bound
emission (inset of Fig. 4).
Figure 5 shows raw data recorded using a Static X-ray Imager
(SXI)39,40 pinhole CCD camera, which is filtered to observe 3–5 keV
x-rays. The lower signal in the Ti image is consistent with free–bound
dominated emission, which is largely filtered by the SXI due to the
K-series limit being just above the sensitivity range. The strong
FIG. 5. X-ray emission spot images and widths for Au, Au, Ag, and Ti recorded
using SXI. False-colored raw data for each shot is shown along the top. The nomi-
nal laser intensity pattern (1 mm FWHM) and view from SXI are shown in the
inset (crooked due to view). Vertically averaged lineouts from the highlighted region
in each image across the top are shown in the main figure; the lineouts are normal-
ized and offset. The FWHM of a Gaussian fit is written below the corresponding
raw image and represented by lines drawn at the bottom of the main figure.
Appl. Phys. Lett. 117, 251106 (2020); doi: 10.1063/5.0033629
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bound–bound emission from Au and Ag in this regime accounts for
the higher signal levels. This is consistent with previous results com-
paring matched K- and L-shell emission at similar ne and Te.41
In the raw SXI images (Fig. 5), the vertical and horizontal direc-
tions correspond roughly to foil normal and transverse directions,
respectively. The Au vertical spot size is 35% larger than Au, consis-
tent with pre-expansion by the picket. We do not observe a significant
difference across picketed pulse shape experiments, suggesting
material independent expansion. The keV x-ray transverse emission
volume also yields clues about the interplay between conduction out
of the heated region and radiative losses. Thermal conductivity in the
Lee–More [LM] model42 scales as / ne Te5=2 =Z  . For constant Te and
ne, the LM thermal conductivity decreases with increasing Z. The com-
bined lower radiative losses and higher conductivity are consistent
with the larger emission size observed for decreasing Z.
In conclusion, we have observed 4X stronger multi-keV contin-
uum x-ray emission from Ti than Ag or Au. The extraordinary energy
density produced by the NIF lasers ionizes Ti samples into the K-shell,
causing strong continuum emission from free–bound transitions.
X-ray spectrometer data show direct evidence for both large free–
bound emission enhancement in Ti and a significant population of
hydrogen-like Ti atoms. Our conclusions are well-supported by ana-
lytical scaling, radiation-hydrodynamics simulations, and detailed
spectroscopic calculations. Despite strong continuum emission, Ti has
lower overall radiative losses due to fewer bound–bound transitions
that dominate emission from high-Z atoms. This combined with ther-
mal conductivity produces an emission volume that scales inversely
with Z, further enhancing Ti continuum emission. The continuum
spectral slopes suggest that Te scales positively with Z due to a combi-
nation of increasing IB laser absorption and reducing thermal conduc-
tivity. In agreement with previous studies, we find that a picketed laser
pulse shape increases the laser absorption efficiency. It may be possible
to achieve higher free–bound contributions in higher-Z materials by
taking advantage of the large number of potential vacancies in the L-
shell. Achieving this would require higher Te that might be possible
using magnetic fields.43,44 Additionally, initially sub-critical density
targets (gas or foam) also produce very intense x-ray pulses,14,16,17 but
material availability for these types of samples is limited, and at a size
of 4 mm, they are quite large and may not be practical for all
applications.
See the supplementary material for the details that further
describe our results. The first part includes information about the NSS
and Virgil x-ray spectrometers. The second part are technical details
about the hydrodynamics simulations.
This work was performed under the auspices of U.S.
Department of Energy by the Lawrence Livermore National
Laboratory under Contract No. DE-AC52-07NA27344. This
document’s release number is: LLNL-JRNL-817453. This document
was prepared as an account of the work sponsored by an agency of
the United States government. Neither the United States
government nor the Lawrence Livermore National Laboratory,
LLC, nor any of their employees makes any warranty, expressed
or implied, or assumes any legal liability or responsibility for
the accuracy, completeness, or usefulness of any information,
apparatus, product, or process disclosed, or represents that its use
117, 251106-4
 Applied Physics Letters
would not infringe privately owned rights. Reference herein to any
specific commercial product, process, or service by trade name,
trademark, manufacturer, or otherwise does not necessarily
constitute or imply its endorsement, recommendation, or favoring
by the United States government or Lawrence Livermore National
Security, LLC. The views and opinions of the authors expressed
herein do not necessarily state or reflect those of the United States
government or Lawrence Livermore National Security, LLC, and
shall not be used for advertising or product endorsement purposes.
DATA AVAILABILITY
The data that support the findings of this study are available
from the corresponding author upon reasonable request.
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