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Photoluminescence-Tunable Carbon Nanodots:
Surface-State Energy-Gap Tuning
Lei Bao, Cui Liu, Zhi-Ling Zhang, and Dai-Wen Pang*
Luminescent nanoparticles, such as semiconductor quantum
dots (QDs)[1,2] and metal nanoclusters[3,4] offering unique
photophysical characteristics, have dramatically changed the
paradigm of fluorescence in the past years. Among them,
carbon nanodots (C-dots)[5] – with their high photostability,
good biocompatibility, and facile preparation – are promising
substitutes for the present fluorescent nanomaterials of various
applications, such as biomedical imaging,[6–8] analyte detec-
tion,[9–11] and light-emitting devices.[12–14] Typically, a C-dot of
less than 10 nm has an sp2 or amorphous carbon framework
and a surface coated with oxygen-containing groups, polymers,
or other species.[15,16] To date, the preparations for C-dots gener-
ally include laser ablation,[17,18] electrochemical oxidation,[19–21]
carbonization,[22,23] wet oxidation,[24,25] ultrasound,[26] and
microwave-assisted synthesis.[27] Reports on this topic are con-
tinuously increasing. Nonetheless, the properties of fluorescent
C-dots remain largely unexplored. One crucial issue is whether
C-dots can be engineered, like quantum dots, so as to tune
their luminescence. This challenge is due to a lack of suffi-
cient theoretical and experimental knowledge on C-dots; there-
fore, it is imperative that we understand the origins of their
photoluminescence (PL) , and that we subsequently develop
a rational strategy to tune their PL properties for multicolor
imaging applications. Herein, we reveal that the fluorescence of
C-dots originates from surface-state emission, where the energy
gap is governed by the surface properties and size of the C-dots.
Accordingly, we demonstrate that a series of C-dots exhibiting
various colors of fluorescence can be prepared by varying their
degree of surface oxidation or their size. The prepared C-dots
have potential for application in multicolor imaging.
The synthesis of fluorescent C-dots was achieved through
the oxidation of carbon fibers (CFs) in nitric acid followed by
ultrafiltration. Three effectively separated fractions with molec-
ular weights equivalent to <3, 3–10, and 10–30 kDa were col-
lected; they are denoted as C-dots(<3k), C-dots(3–10k), and
C-dots(10–30k), respectively. The high-resolution transmis-
sion electron microscopy (HR-TEM) images of the C-dots
(Figure 1A–C) illustrate their uniformity and good dispersion,
with diameters of 2.7 ± 0.4, 3.3 ± 0.6, and 4.1 ± 0.6 nm for
Dr. L. Bao, C. Liu, Prof. Z.-L. Zhang, Prof. D.-W. Pang
Key Laboratory of Analytical Chemistry for Biology
and Medicine (Ministry of Education)
College of Chemistry and Molecular Sciences
State Key Laboratory of Virology, the Institute for
Advanced Studies and Wuhan Institute of
Biotechnology
Wuhan University
Wuhan 430072, PR China
E-mail: dwpang@whu.edu.cn
DOI: 10.1002/adma.201405070
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DOI: 10.1002/adma.201405070
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C-dots(<3k), C-dots(3–10k), and C-dots(10–30k), respectively.
The X-ray diffraction (XRD) patterns of the C-dots (Figure 1D)
were obtained to identify their crystalline nature. The diffrac-
tion peaks with 2θ values of 23.9° and 40.4° corresponded to
the 002 and 100 facets, respectively, of graphite (powder diffrac-
tion file (PDF) No. 65–6212). The Fourier-transform IR (FTIR)
spectra of the C-dots (Figure 1E) suggested abundant oxygen-
containing groups on their surfaces; such groups include
hydroxyl (v(O–H), 3428 cm−1), carboxyl (v(C=O), 1743 cm−1),
and carbonyl (v(C=O), 1630 cm−1) groups. Additionally, Raman
spectroscopy was utilized to characterize the intrinsic struc-
ture of the C-dots (Figure 1F). Common features were present
in the 1000–2000 cm−1 region, where the G band peaking at
1590 cm−1 indicates sp2 carbon networks and the D-band
peaking at 1350 cm−1 reflects the disorder or defects in the
graphitized structure. The intensity ratios of the D- to G-bands
(ID/IG) for C-dots(<3k), C-dots(3–10k), and C-dots(10–30k) were
0.98, 0.85, and 0.84, respectively. The existence of a large frac-
tion of defects mainly resulted from surface oxidation, which is
consistent with the FTIR results.
The PL properties of the as-prepared C-dots were investi-
gated. All types of C-dots herein emitted at fluorescence wave-
lengths independent of the excitation wavelengths (Figure S1,
Supporting Information). Such a characteristic indicates that
predominant emissive sites with maximum transition prob-
ability on the C-dots were generated under vigorous oxidation.[28]
This feature of excitation-independent PL makes the prepared
C-dots more likely to be applicable to bio-imaging applications.
Additionally, the emissions of the C-dots gradually red-shifted as
a result of prolonged oxidation time. As illustrated in Figure 2A,
the peak wavelength of C-dots(<3k) moved from 430 to 520 nm,
that of C-dots(3–10k) moved from 505 to 570 nm, and that of
C-dots(10–30k) moved from 510 to 610 nm. To verify the involved
mechanism, we analyzed C-dots(<3k) obtained at various oxida-
tion times in detail. The TEM and XRD results (Figure S2A–E,
Supporting Information) revealed that C-dots(<3k) obtained
at various oxidation times had identical crystalline structures
and a size of 2.7 nm. Their surface characteristics were inves-
tigated by C 1s high-resolution X-ray photoelectron spectros-
copy (XPS) spectra (Figure 2B); the following contribution
could be assigned: graphitic carbons (sp2, 284.5 eV), alcoholic
carbons (C–O, 286 eV), carbonyl carbons (C=O, 287.8 eV), and
carboxyl carbons (O–C=O, 289 eV). For the C-dots obtained at
6 to 48 h (denoted as C-dots(6h <3k), C-dots(48h <3k), etc.),
the relative intensity of the C 1s XPS peak in the range of
286–289 eV increased, and the peak gradually shifted towards
the high binding-energy side, implying a rise in the percentage
of oxygen-containing groups. The quantitative analysis also sug-
gested that the oxygen-to-carbon ratio increased from 0.52 to
0.67, that carbonyl-group content increased from 10% to 20%,
and that the carboxyl-group content increased from 3% to 6%.
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Figure 1. A–C) HR-TEM images of C-dots(<3k) (A), C-dots(3–10k) (B), and C-dots(10–30k) (C) obtained via oxidation of CFs (0.15 mg) in aqueous
HNO3 (5 M) for 48 h. D) XRD patterns, E) FTIR spectra, and F) Raman spectra of the indicated C-dots.

It has been revealed that surface defects created by surface
oxidation serve as capturing centers of excitons, thereby giving
rise to the surface-state-related fluorescence.[20,27] The higher
the surface oxidation of the C-dots, the more surface defects
are present on the C-dots. Such a change consequently nar-
rows the energy levels and causes the red-shifted fluorescence
emission of the C-dots.[29] Thus, the fluorescence peak of the
resulting C-dots moved to longer wavelengths as the duration
of oxidation increased. This behavior is consistent with pre-
vious work,[29] suggesting surface-oxidation-related fluores-
cence. As a result of this characteristic, the optical properties
of C-dots can be tuned without changing their particle size.
Additionally, owing to more surface emissive sites created via
increasing the oxidation time, the brightness of C-dots can be

Figure 2. A) Time evolution of PL peak wavelengths of C-dots. The standard deviation of wavelengths was less than 10 nm. CHNO3, T, and mCFs rep-
resent the nitric acid concentration, temperature, and the mass of the carbon fibers, respectively. B) C 1s high-resolution XPS spectra of C-dots(<3k)
obtained at indicated reaction times. C) UV–vis and PL spectra (excitation wavelength was 360 nm) of C-dots(48h <3k), C-dots(48h 3–10k), and
C-dots(48h 10–30k). D) ECL spectra of C-dots(9h <3k), C-dots(48h <3k), C-dots(48h 3–10k), and C-dots(48h 10–30k) as indicated. The standard devia-
tion of the ECL peak value is 20 nm. Inset: Schematic of the proposed mechanism for PL and ECL of C-dots.

2 wileyonlinelibrary.com © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Adv. Mater. 2015,
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increased.[30] The fluorescence quantum yields (φ) of C-dots sig-
nificantly increased from 1.1% to 20.7% with longer reaction
times (Figure S2F, Supporting Information).
Moreover, we noticed that the peak wavelength of C-dots
obtained at a given time displayed a red-shift as larger
C-dots were considered. Taking C-dots obtained at 48 h as an
example (Figure 2C), the peak wavelength was 526 nm for
C-dots(48h <3k), 570 nm for C-dots(48h 3–10k), and 608 nm
for C-dots(48h 10–30k). This trend indicates that not only the
surface oxidation but also the size of the C-dots have influence
on the emission wavelength of the prepared C-dots. Some sug-
gestions have attributed this phenomenon to the conjugate
effect[21,31] or quantum-size effect;[19] nevertheless the mecha-
nism remains an open question. It is known that the emis-
sion wavelength of photoluminescent materials is related to
the energy gap between excited states and the ground state,[32]
while energy levels of the electronic states are determined by
the intrinsic electronic structure of the materials. The UV–vis
absorbance peak for the C-dot π–π* transition (ca. 228 nm;
Figure 2C) implied the existence of a large π-electron system.
This π-electron system can strongly couple with surface elec-
tronic states created by the surface oxidation, consequently
altering the overall electronic structure of the C-dots.[33] To elu-
cidate the mechanism of this effect, the radiative (kr) and non-
radiative (knr) rate constants were determined using the time-
resolved photoluminescence (TRPL) technique (Table S1, Sup-
porting Information). Given that the average lifetime (τaverage)
of C-dots is ca. 2 ns, the fluorescence radiative rate constant
(kr = φ/τaverage) was calculated to be on the order of 107 s−1,
which is 10 times slower than that of bandgap-like fluores-
cence emitted by polymers functionalized C-dots.[34] Also,
based on the relationship: φ = kr/(kr + knr), the non-radiative
rate constant of C-dots was calculated to be on the order of
108 s−1, which is comparable to the fast non-radiative process
observed on their counterparts of Si nanoparticles.[33] These
recombination processes are related to the electronic transi-
tions in the C-dots, indicating the strong coupling between the
core and surface sates.[35] In terms of that, we speculate that
the change in the extent of the π-electron system affects the
energy levels of the surface electronic states. An increase in
the extent of the π-electron system will lower the energy gap
of the π–π* transitions and further result in a small energy
gap for the surface states. Therefore, large C-dots possessed
long-wavelength fluorescence. However, the large C-dots have
fewer surface defects (Figure 1F). Due to surface-state emission
nature,[30] fluorescence quantum yields of the C-dots decreased
from 20.7% to 4.5% to 1.8% for C-dots(<3k) to C-dots(3–10k) to
C-dots(10–30k).
Furthermore, electrogenerated chemiluminescence (ECL)
spectroscopy, which is a highly sensitive technique for probing
the surface of nanoparticles,[36] was employed to probe the
surface-state electronic transitions of the C-dots. As shown in
Figure 2D, the ECL spectra of C-dots(9h <3k), C-dots(48h <3k),
C-dots(48h 3–10k), and C-dots(48h 10–30k) peaked at 465, 530,
570, and 608 nm, respectively. Each ECL peak was very close
to its corresponding PL peak, indicating that the PL of C-dots
most likely emitted from the same surface emissive sites as the
ECL of the C-dots[37] (Figure 2D, inset). Additionally, we consid-
ered case I, in which C-dots of the same size but have different
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surface chemistry, e.g., C-dots(9h <3k) and C-dots(48h <3k) and
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case II, in which the C-dots have different core sizes but the
same reaction time, e.g., C-dots(48h <3k), C-dots(48h 3–10k),
and C-dots(48h 10–30k). It is notable that in case I, where the
same-sized C-dots increased in the surface-oxidation degree as
the reaction time increased, the ECL spectrum shifted from
465 to 530 nm). Meanwhile in case II, where the core size of
the C-dots increased, the ECL spectrum was also red-shifted.
These features disclose that changes in the surface chemistry
or π-electron system of the C-dots have significant influence on
the energy gaps of the surface states. The higher the surface
oxidation or the higher the extent of the π-electron system, the
smaller the energy gap of the surface states in the C-dots. Based
on these observations, we assert that the PL of the C-dots is of
surface-state emission and that the energy gap of the surface
emissive sites is a function of both the π-electron system and
the surface chemistry. As a result, by controlling their size and
surface characteristics, C-dots with desired PL properties can be
accordingly engineered.
To demonstrate the above proposal, we conducted systemic
experiments on how the PL of C-dots change with their size
and surface chemistry. In the synthetic approach, those two
elements (size and surface) were controlled by reaction time,
concentration of HNO3, and reaction temperature. The PL evo-
lution of the C-dots with different reaction conditions is avail-
able in the Supporting Information (Figure S3). The results
are summarized as follows: i) Prolonging the reaction time
increased the surface oxidation and resulted in longer emission
wavelengths. ii) Higher concentrations of HNO3 for the reac-
tion resulted in longer emission wavelength for short reaction
times. For instance, the fluorescence of the C-dots was 435 nm
after 6 h of reaction at 2.5 M HNO3 (denoted as C-dots(6h <3k,
2.5M)), while it can reach 515 nm after 6 h of reaction at 7.5 M
HNO3 (denoted as C-dots(6h <3k, 7.5M)). Further characteri-
zation of the resulting C-dots by TEM (Figure S4, Supporting
Information) showed that the diameters of C-dots(6h <3k,
2.5M) and C-dots(6h <3k, 7.5M) were 2.5 ± 0.5 and 3.0 ± 0.5 nm,
respectively. This implied that the concentration of HNO3
determines the formation of fluorescent C-dots. At low concen-
trations of HNO3, exfoliation may start from the defect sites
on the CFs, preferentially forming smaller C-dots while larger
C-dots tended to be formed at high concentrations of HNO3.
Moreover, higher concentrations of HNO3 may result in a
higher degree of surface oxidation, further facilitating C-dots
with long-emission wavelengths. iii) Blue and green lumines-
cent C-dots more preferentially formed at low temperature
while C-dots with longer emission formed at high tempera-
ture for short reaction times. It is possible that the oxidizing
capacity of nitric acid is weakened at low temperature, resulting
in C-dots with a low degree of surface oxidation and a short flu-
orescence wavelength.
Diagrams of these results provided a comprehensive
experimental guide to the synthesis of C-dots with certain
PL properties. Based on the diagrams, a series of excitation-
independent fluorescent C-dots with emission wavelengths
ranging from 430 to 610 nm were prepared accordingly.
(Figure 3A). Under the excitation of blue light, the entire
series of the as-prepared C-dots synchronously emitted
fluorescence at each of their fluorescence wavelengths,
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Figure 3. A) Top: Optical images of as-prepared multicolor fluorescent a) C-dots(6h <3k, 2.5M), b) C-dots(9h <3k, 5M), c) C-dots(6h <3k, 7.5M),
d) C-dots(6h 10–30k, 7.5M), e) C-dots(48h 3–10k, 5M), f) C-dots(24h 10–30k, 5M), and g) C-dots(48h 10–30k, 5M). Bottom: Fluorescence emission
spectra of C-dots in (a) to (g) from left to right, with excitation at 360 nm. B) Microscopic images of Vero cells with internalized green C-dots (b,d),
yellow C-dots (e,g), and red C-dots (f,h). The control experiments were Vero cells without internalized C-dots (a,c). Images for (a,b,e,f) were taken in
the bright field, and images for (c,d,g,h) were taken in the fluorescent field.

demonstrating the prospect of applying C-dots to multicolor
imaging. In addition, it is anticipated that increased bright-
ness in the fluorescence can be obtained by generating more
defects on their surface.[6] The fluorescence-tunable C-dots
exhibiting the major merits of broad absorption, simulta-
neous excitation by one wavelength, high photostability, and
low toxicity (Figure S5, Supporting Information) have signifi-
cant potential for bio-imaging applications. As illustrated in
Figure 3B, three kinds of prepared C-dots with green, yellow,
and red fluorescence were spontaneously incorporated into
cultured Vero cells, which might be ascribed to an endocy-
tosis mechanism.[38] Further efforts devoted on the surface
functionalization of C-dots, preparation of C-dots with narrow
full-width-at-half-maximum (FWHM) values, and enhance-
ment of their fluorescence quantum yields will certainly ben-
efit the application of multicolor C-dots as alternative probes
for fluorescence-based multitasks, such as high-throughput
screening or multicolor coding.
In summary, a controllable wet oxidation method for synthe-
sizing excitation-independent C-dots with tunable fluorescent
colors has been developed. Significantly, using surface analyt-
ical techniques, time-resolved photoluminescence spectroscopy,
and the ECL technique, we have revealed that the PL properties
of C-dots, mainly influenced by their size and degree of surface
oxidation, can be tuned by varying reaction time, temperature,
and concentration of nitric acid. The energy gap of the surface
states, where electrons and holes recombine to emit fluores-
cence, correlated with the extent of the π-electron system and
surface chemistry. This work offers a new insight into C-dots
from the viewpoints of both experiments and mechanism,
which will promote diverse applications of C-dots in the near
future.
Experimental Section
Synthesis: CFs (0.15 g) were added to a nitric acid solution (30 mL,
5 M). Then, the well-stirred solution was heated to 120 °C and refluxed
for 48 h. The corresponding solution containing C-dots was collected
at a given time (e.g., 6, 8, 12, 24, 36, and 48 h) and then neutralized
with NaOH. The resulting solution was first filtered by BIOSHARP
membrane filters (0.22 µm) and then ultrafiltered successively through
Millipore centrifugal filter devices with four different molecular-weight
cut-off (MWCO) membranes (i.e., 30, 10, and 3 kDa). Accordingly, the
effectively separated fractions with weights equivalent to <3, 3–10, and
10–30 kDa were collected and further dialyzed for the analysis.
ECL Measurements: The ECL experiments were conducted in a three-
electrode electrochemical system with a Pt-disk working electrode, a
Pt-wire counter electrode, and an Ag/AgCl reference electrode. By using
cyclic voltammetry with the potential sweeping between 0 and −1.5 V
at a scan rate of 0.5 V s−1, ECL signals of the C-dots (0.2 mg mL−1) in
the electrolyte containing phosphate buffer solution (PBS) (0.1 M, pH
7.4), K2S2O8 (1 mM), and Na2SO4 (0.5 M) were obtained and collected
simultaneously by the photomultiplier tube (PMT) biased at 900 V. The
ECL spectra of the C-dots were measured by collecting the various ECL
intensities at −1.5 V with band-pass filters at the wavelengths of 400,
420, 450, 470, 490, 510, 535, 570, 590, 610, 630, 645, 665, 695, 715 and
730 nm used in the detection system; afterward, the difference of the
ECL intensities were plotted with the corresponding wavelength.

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DOI: 10.1002/adma.201405070

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Supporting Information
Supporting Information is available from the Wiley Online Library or
from the author.
Acknowledgements
This work was supported by the National Basic Research Program of
China (973 Program, No. 2011CB933600), the Program for New Century
Excellent Talents in University (NCET-10–0656), and the 111 Project
(111–2–10). L.B acknowledges a 2014 Endeavour Fellowship. The
authors would also like to thank Mr. En-Ze Sun for his help with the
cytotoxicity experiment; Prof. Cheng-Zhi Huang and Ms. Lin-Ling Zheng
for their assistance of the PL lifetime experiments; and Mr. Yi-Wei Hu for
helpful suggestions.
Received: November 5, 2014
Revised: November 28, 2014
Published online:
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