COMMUNICATION
Photochromic Memory
Light-Tunable Nonvolatile Memory Characteristics in
Photochromic RRAM
Haifeng Ling, Kangming Tan, Qiyun Fang, Xinshui Xu, Hao Chen, Wenwen Li, Yefan Liu,
Laiyuan Wang, Mingdong Yi, Ru Huang, Yan Qian,* Linghai Xie,* and Wei Huang*
Light-tunable resistive switching (RS) characteristics are demonstrated in
a photochromophore (BMThCE)-based resistive random access memory.
Triggered by nondestructive ultraviolet or visible light irradiation, two
memory-type RS characteristics can be reversibly modulated in the same
device upon a narrow range of applied voltage (<6 V), accompanied by the
photochromophores in the active layer reversibly changed between ring-open
state (namely, o-BMThCE) and ring-closed state (namely, c-BMThCE). The
o-BMThCE-based memory exhibits a write-once-read-many characteristic with
a high current on/off ratio of 105, while the c-BMThCE-based one shows a
flash characteristic. Both of the RS characteristics present good nonvolatile
stability with the resistance states maintained over 104 s without variation.
This RS modulation is possibly related to the formation and rupture of con-
ductive filaments, which formed along channels consisting of BMThCE trap-
ping molecules. This work provides a new memory element for the design of
light-controllable high density storage and data encryption technology.
Resistive random access memory (RRAM) technology has
emerged as an attractive candidate for next-generation
Dr. H. F. Ling, K. M. Tan, Q. Y. Fang, X. S. Xu, H. Chen, W. W. Li,
Dr. L. Y. Wang, Prof. M. D. Yi, Prof. Y. Qian, Prof. L. H. Xie,
Prof. W. Huang
Key Laboratory for Organic Electronics and Information
Displays (KLOEID)
Institute of Advanced Materials (IAM)
Jiangsu National Synergetic Innovation Center for
Advanced Materials (SICAM)
Nanjing University of Posts and Telecommunications
9 Wenyuan Road, Nanjing 210023, China
E-mail: iamyqian@njupt.edu.cn; iamlhxie@njupt.edu.cn;
iamwhuang@njupt.edu.cn, iamwhuang@njtech.edu.cn
Dr. Y. F. Liu, Prof. R. Huang
Institute of Microelectronics
Peking University
5 Yiheyuan Road, Beijing 100871, China
Prof. W. Huang
Key Laboratory of Flexible Electronics (KLOFE)
Institute of Advanced Materials (IAM)
Jiangsu National Synergetic Innovation Center for
Advanced Materials (SICAM)
Nanjing Tech University
30 South Puzhu Road, Nanjing 211816, China
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/aelm.201600416.
DOI: 10.1002/aelm.201600416
Adv. Electron. Mater. 2017, 1600416 1600416  (1 of 7)
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nonvolatile memory due to its excel-
lent miniaturization potential (<10 nm),
high switching speed (sub-ns), high
data storage density (4F2/n), and high
cycling endurance (>1012).[1,2] Based on
the change of switchable resistance states
of the active layer, RRAM has excel-
lent tunability to deliver a wide variety
of memory-type (flash, write-once-read-
many (WORM), the static random access
memory (SRAM), or the dynamic random
access memory (DRAM)) or threshold-
type resistive switching (RS) elements for
the complementary metal oxide semicon-
ductor (CMOS) technology, such as 1D–1R
cell array or neuromorphic circuits.[3] The
modulation strategies of various memory-
type RS include tuning of molecular struc-
tures,[4,5] film thickness or morphology
of the active layer,[6,7] dopants or doping
level in composites or matrixes,[8] and
electrode materials,[9] etc. These strategies usually require two
or more controlling devices, which correspondingly exhibit dif-
ferent memory behaviors. However, a single integrated multi-
functional memory cell is essential for device miniaturization
and portable circuit systems. To date, the modulation of RRAM
to display dual- or multi-RS characteristics within a single
device has been rarely reported. Recently, by tuning the com-
pliance current (Icc), switching between nonvolatile memory
(at high Icc) and volatile threshold characteristic (at low Icc) has
been demonstrated in one device.[10,11] By increasing UV irra-
diation time, irreversible tuning from unswitchable high resist-
ance state to switchable WORM- and flash-type memory, and
ultimately unswitchable low resistance state can be achieved.[12]
However, to the best of our knowledge, nondestructive and
reversible modulation between different nonvolatile memory-
type RS has not been reported yet.
Compared to electrical tuning, light controlling has emerged
as a facile and low-power stimuli which enables nondestructive
programming of resistive switching behavior, by converting
light information into electric response.[13] In addition, a com-
bination of bias voltage-tuning and light-tuning could broaden
the device function and allows multifunctional and highly inte-
grated nanodevices and/or sensors, such as multibit storage,[14]
data encryption technology,[15] or neuromorphic sensing plat-
forms.[16] Moreover, light tuning provides good model systems
to study the memory mechanism, which remains controversial
in organic memories. In this regard, organic photochromic
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materials have attracted considerable atten-

tions for various light-assisted memory
applications.[17–19] Among them, diaryl­
ethenes (DAEs) are well known as a series
of photochromic molecules with excellent
thermal stability and high fatigue resistance
in reversible isomerization.[17,20,21] By light
irradiation at appropriate wavelengths, the
photochromophores undergo a reversible
photochemical transformation between the
ring- open and closed isomers, accompa-
nied by the reversible changes of both optical
(absorption/fluorescence, refractive index,
etc.) and electrical (the highest occupied
molecular orbital (HOMO)/ the lowest unoc-
cupied molecular orbital (LUMO)), carrier
mobility, conductivity, etc.) properties.[18,22,23]
As a result of the above changes, two dis-
tinct states can be defined as “0” and “1”,
respectively, as information bits in a digital
memory.[17,18] This memory characteristic has
been demonstrated in optical recording,[18]
molecular switch,[23,24] photocontrollable
or photoswitchable transistors,[25] organic
memory transistors,[14,26,27] diode memo-
ries,[20,28,29] memorizable photochromic light-
emitting diodes,[21,30] and so on.
In this work, by using a DAE derivative
(BMThCE) as the active layer, we reported a
single photochromic RRAM which exhibited
reversible switching between nonvolatile
flash and WORM characteristics. Triggered
by nondestructive ultraviolet or visible light
irradiation, the two memory-type RS char-
acteristics have been demonstrated at low
applied voltages (<6 V), caused by trap-depth
tuning due to reversible photochromism Figure 1.  a) Schematic diagram of BMThCE-based memory, and the chemical structures of the
between ring-open state (namely o-BMThCE) photochromic diarylethene (UV: ultraviolet light; VIS: visible light). I–V characteristics of the
BMThCE-based memories: b) ITO/o-BMThCE/Al, and c) ITO/c-BMThCE/Al. And continuous
and ring-closed state (namely c-BMThCE). bias stress measurements at 0.5 V: d) ITO/o-BMThCE/Al, and e) ITO/c-BMThCE/Al.
The o-BMThCE isomer-based memory
exhibits a WORM characteristic with a high
current on/off ratio (OOR) of 105, while the c-BMThCE isomer- abruptly switched to the low resistance state (LRS, 2.7 × 102 Ω)
based device shows a flash characteristic. Both of the RS char- at the turn-on voltage (VSET) of 2.7 V (in Sweep 1). This HRS-to-
acteristics present good nonvolatile stability with the resistance LRS transition was equivalent to the SET operation in a digital
states maintained over 104 s without variation. memory. Then the LRS could be maintained during the sub-
Figure 1a shows the schematic diagram of the ITO/ sequent sweeps (Sweep 2–8) even after removal of the applied
BMThCE (30 nm)/Al (100 nm) memory device. The as-depos- voltage, indicative of a WORM type characteristic. The current
ited BMThCE molecules were normally the ring-open iso- OOR was higher than 105 (read at 0.5 V), which is a consid-
mers (o-BMThCE), which converted to the ring-closed isomers erable magnitude in the two-terminal photochromic memo-
(c-BMThCE) under the trigger of UV irradiation (I0 = 2.49 mW ries.[31] Then, under UV light irradiation, the device based on
−2
cm at λ = 200–400 nm). When the c-BMThCE molecule was photostationary ring-closed photochromophores has been
subject to visible-irradiation (I0 = 5.86 mW cm−2 at λ > 490 nm), achieved (denoted as ITO/c-BMThCE/Al). The I–V curve of the
it could recover to the initial open state. The reversible trans- c-BMThCE-based memory was shown in Figure 1c. During the
formation between o-BMThCE and c-BMThCE can be achieved first sweep from 0 to 6 V, a SET process was observed at ≈1.0 V
by alternative UV and visible light illumination, as demon- from HRS (2.5 × 104 Ω) to LRS (1.3 × 102 Ω). When the applied
[26]
strated in our previous work. For the original ring-open state voltage was swept to negative bias, the resistance increased
(denoted as ITO/o-BMThCE/Al, Figure 1b), when a positive abruptly from the LRS (1.3 × 102 Ω) to HRS (4.0 × 104 Ω)
voltage sweep was applied from 0 to 6 V, the device was ini- at turn-off voltage (VRESET) of −4.0 V, corresponding to the
tially in a high resistance state (HRS, 6.1 × 107 Ω) and then RESET operation. In the subsequent fifth to eighth sweeps, the

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Figure 2.  Energy band diagrams and memory characteristics of the BMThCE-based memories (Left: ITO/o-BMThCE/Al; Right: ITO/c-BMThCE/Al):
a,b) Energy band diagrams; c,d) Experimental and fitted I–V curves of HRS and LRS; e,f) Device area dependent- resistances and temperature-
dependent currents of HRS and LRS (both read at 0.5 V); g,h) The transient response of the memories. A 50 V read resistor was in parallel with an
oscillography to record the device response.

alternate transition between HRS and LRS could be performed
again, showing a typical flash characteristic with the OOR of
103 (readout at 0.5 V). Moreover, for both RS characteristics,
no significant degradation was detected in the LRS and HRS
during 3 h of the continuous bias stress at 0.5 V (Figure 1d,e),
demonstrating good nonvolatile stability.
It was notable that the o-BMThCE-based memory showed
higher OOR due to the higher resistance in HRS (RHRS). The
RHRS for o-BMThCE-based memory was 7.3 × 106 Ω at 0.5 V,
nearly 2 orders of magnitude higher than that of the c-BMThCE-
based one (1.0 × 105 Ω). The higher RHRS originated from the
larger hole injection barrier between ITO and o-BMThCE. As
illustrated in Figure 2a,b, the hole injection barrier between
ITO and o-BMThCE/c-BMThCE is much smaller than the elec-
tron injection barrier, indicating that hole carriers dominate
the injection from ITO to the HOMO level of the BMThCE in
both memories. The c-BMThCE showed a higher HOMO level
(−4.95 eV) than that of the o-BMThCE (−5.32 eV), which facili-
tated the hole injection and transportation. However, the resist-
ances of LRS (RLRS) of both o-BMThCE- and c-BMThCE-based
memory were in the same order of magnitude (≈102 Ω at 0.5 V),
revealing the independence of hole injection barrier when in

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the LRS and a possible generation of localized conducting path.
Besides, for the c-BMThCE memory, the second SET operation
(Sweep 5) appeared at a more positive voltage of 4.5 V than that
in the first SET operation (Sweep 1, 1.0 V), showing a wide VSET
distribution (Figure S1, Supporting Information), which is a
typical feature of the random reformation of conductive fila-
ments (CFs).[31,32] Therefore, we speculated that the formation
of CFs should be responsible for the LRS in the present work.
To investigate the switching and conduction mechanism,
LRS and HRS of both memories were fitted, respectively. For
the HRS of o-BMThCE memory (inset of Figure 2c), a plot
of ln(I/V) versus V1/2 was linearly fitted with a slope of ≈2.6,
indicative of a charge trap related Poole–Frenkel (PF) emis-
sion mechanism.[33] While for the HRS of c-BMThCE memory
(Figure 2d), the carrier conduction is dominated by a typical
trap-controlled space-charge-limited current (SCLC) model
which consisted of three regions: (1) an Ohmic conduction
(I ∝ V) with a slope of ≈1.0 in the initial low voltage region,
(2) a SCLC obeying the Child law (I ∝ V2) with the slope of 2.0
in the middle region, and (3) a trap-free SCLC (I ∝ Vk, k > 2)
where the slope is ≈6.8.[32] Although the two memories showed
different conduction behaviors in HRS, it is indicated that both
the HRSs are related to charge traps of the switching layer.
However, for the LRS of two memories, the linear plot of log
(I) versus log (V) with a slope ≈1.0 was suitable for the Ohmic
conduction, signifying a conductive filament-based switching
mechanism.[34]
The dependences of device area and operation temperature
on resistance switching properties were investigated to further
confirm the conduction mechanism and the CFs composition.
Both the area- and temperature-dependent measurements are
well consistent with the fitted results of I–V curves that the
resistance switching mechanism involves trap-assisted fila-
ments formation. For the o-BMThCE memory device, when the
device area decreased from 2.5 × 105 (500 × 500) to 104 (100 ×
100) µm2, the RHRS increased from 7.4 × 106 to 1.6 × 108 Ω
(Figure 2e; and Figure S2, Supporting Information). RHRS
nearly exhibited a linear decreasing dependence as the func-
tion of device area, indicating that HRS currents (IHRS) flowed
through the whole device area. In contrast, the resistance in
the LRS (RLRS) showed negligible dependence on the device
area, which is a typical CF feature that the current value of
the LRS (ILRS) is determined by localized conductive path.[35,36]
Similar behaviors were observed in c-BMThCE-based memory
devices (Figure 2f; and Figure S3, Supporting Information).
The temperature-dependent measurements showed the Arrhe-
nius behavior of IHRS and ILRS as a function of 1/T (Figure 2e,f,
derived form Figures S4 and S5, Supporting Information). For
both devices, the ILRS was almost temperature-independent,
indicative of tunneling transport through filamentary path.[37,38]
This is against the typical feature of metallic CFs in which the
LRS current should exhibit a decreasing trend when tempera-
ture increases.[36,39] However, the IHRS increased almost linearly
with increasing the temperature (from 25 to 100 °C), indi-
cating a thermally activated transport with an activation energy
(ϕ) of ≈60 meV for c-BMThCE-based device and ≈94 meV for
o-BMThCE-based device, respectively.[32,38] The smaller ϕ value
of c-BMThCE memory device indicated that there exist shal-
lower traps in the c-BMThCE switching layer when at HRS.
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In our devices, a preforming operation with high “+” ve
to the active metal electrode is not required, precelding the
metallic filament mechanism.[40] In addition, the RLRS in our
devices (130–251 Ω) is much higher than those in metallic
filament-based memory devices (RLRS < 30 Ω).[4,35,41] Besides,
our memory devices show relatively dispersed SET and RESET
voltage distributions (also see Figure S1, Supporting Informa-
tion). This is also against the carbon-rich filament mechanism,
because carbon-rich filaments are generally highly localized
within only one breakdown region, which leads to a ultrana-
rrow threshold-voltage distribution.[42,1]
Therefore, it is more reasonable that in our cases the
switching behaviors are caused by trap assisted-tunneling fila-
ments rather than the metallic or carbon-rich filaments, indica-
tive of an inherent characteristic of the BMThCE layer. The
resistive switching from HRS to LRS was achieved by charge
tunneling through filament-like paths that consist of charge-
filled traps.[37,43] The trap depths determined by the HOMO
levels of ring-closed or open photochromic molecules are
consistent with the above temperature-dependent measure-
ments.[20,44] Under the applied electric field, the o-BMThCE
(EHOMO = −5.32 eV) and c-BMThCE (EHOMO = −4.95 eV) mol-
ecules then act as deep and shallow charge trapping sites,
respectively. The charge-filled BMThCE traps can serve as step-
ping stones to flow charge carriers.[7] Consistently, the transient
response indicated that the c-BMThCE-based memory with
shallower traps possessed a more rapid switching speed than
the o-BMThCE-based memory with deeper traps (Figure 2g,h).
The effective SET pulses are 4 V/380 ns and 2 V/70 ns for
o-BMThCE and c-BMThCE memories, respectively. The much
faster response of c-BMThCE-based memory indicated that the
ring-closed isomers spatially dispersed in o-BMThCE bulk were
easier to form CFs, with easier filling of the shallow trapping
sites.
Based on the above considerations, we conclude that the
different nonvolatile RS behaviors are attributed to the dif-
ferent depths of the molecular traps in the o-BMThCE- and
c-BMThCE-based memories. In the o-BMThCE-based memory
(Figure 3a–d), the as-deposited BMThCE molecules were nor-
mally the ring-open isomers (o-BMThCE). When the positive
voltage was applied, holes were injected from the bottom ITO
electrode and began to fill the neighboring trapping sites, fol-
lowed by the connection between these sites and thus the
growth of CFs. It is notable that multiple filaments grew simul-
taneously during the voltage sweeping. With gradual increase
of the applied voltage, one of the CFs first reached the top Al
electrode and formed a current percolation path, accounting
for the abrupt transition from HRS to LRS. However, under
the subsequent negative voltage (RESET voltage), the LRS in
o-BMThCE-based memory could not be switched back to the
HRS, due to the deeper trapping sites caused by larger barrier
between o-BMThCE and ITO. Thus, the injected holes were
tightly trapped and, as a result, the WORM type memory was
observed. Intrestingly, by nondestructive UV-light illumination,
the normally irreversible WORM type memory can be switched
to reversible flash type memory. After the device was irradi-
ated by UV light, the generated ring-closed c-BMThCE mole-
cules were quasi-isotropic distributed in the surrounding ring-
open molecules (Figure 3e–h).[28] When the initial voltage was
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Figure 3.  Upper panel: Schematic illustration of the hole injection and transportation in o-BMThCE-based memory: a) Initial state; b) When the posi-
tive voltage is applied, HRS; c) When the applied positive voltage reaches the set voltage, CF is formed, corresponding to LRS; d) When the negative
voltage is applied, still at LRS. Bottom panel: Schematic illustration of the hole injection and transportation in c-BMThCE-based memory. e) Initial
state; f) When the positive voltage is applied, HRS with lower conductivity; g) When the applied positive voltage reaches the SET voltage, CF is formed,
corresponding to LRS; h) When the negative voltage is applied, the CF is broken and the memory switches to HRS.

applied, the inject holes gave priority to fill the shallow traps of The stripe width was 500 µm for both of the patterned ITO (sheet
these ring-closed molecules due to the lower barrier between resistance of 10 Ω/) and Al electrodes. BMThCE was then thermally
evaporated onto ITO to form a 30 nm thick active layer. Finally, about the
c-BMThCE and ITO. Also due to the shallow trapping depth,
100 nm thick Al top electrode was thermally evaporated through a metal
these trapped holes could be easily released under the nega- shadow mask. All deposition processes were carried out in a vacuum
tive voltage. Therefore, the weakly linked CF could be ruptured, of 10−4 Pa. The thicknesses of BMThCE and Al films were measured
and the LRS of the c-BMThCE-based memory switched back to using a Bruker Dektak XT stylus profiler. The electrical properties of the
the HRS, corresponding to a flash type memory. In our cases, memory devices were determined using a Keithley 4200 semiconductor
the flash type memory cannot be obtained simply by reducing characterization system with ITO as the anode at room temperature.
the compliance current.[10] More importantly, these two non- The compliance current was set to be 0.1 A. All these memory behaviors
were investigated in a shielding box.
volatile memory behaviors, i.e., the WORM and flash, can be
reversibly switched under alternative UV and visible light
illuminations (Figure 4).
In summary, light-tunable nonvolatile memory-type RS
characteristics have been integrated in a BMThCE-based
photochromic RRAM. Through nondestructive UV or vis-
ible light irradiation, flash and WORM characteristics could
be reversibly modulated in the same device due to the trap
depth variation. The transition between HRS and LRS can be
explained by the formation and rupture of CF consisting of
ring-closed or open BMThCE molecules. Our approach pro-
vides the design of new prototype of multifunctional organic
photoelectric devices, which exhibits promising potentials
to meet the future trend of downscaling and miniaturizing
memories.

Experimental Section
Materials: The synthesis and full characterization of BMThCE has
been provided in the previous publication.[26]
Device Fabrication and Characterization: The glass/ITO substrate
as one of the electrodes was precleaned in the ethanol, acetone, and Figure 4.  Reversible memory switching processes in a single device. The
deionized water in an ultrasonic bath, each for 10 min in that order. I–V curves were performed under alternative UV and VIS illumination.

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Supporting Information
Supporting information is available from the Wiley Online Library or
from the author.
Acknowledgements
H.F.L. and K.M.T. contributed equally to this work. The authors
express their sincere gratitude to the 973 (2014CB648300) and 863
(2011AA050526) projects, the National Natural Science Foundation
of China (Grant Nos. 21373114, 21573111, and 61475074), a project
funded by the Priority Academic Program Development of Jiangsu
Higher Education Institutions (No. YX03001), Jiangsu National
Synergetic Innovation Center for Advanced Materials (SICAM),
Synergetic Innovation Center for Organic Electronics and Information
Displays, the Minsitry of Education of China (IRT1148), Excellent
science and technology innovation team of Jiangsu Higher Education
Institutions (2013), the Six Peak Talents Foundation of Jiangsu Province
(No. XCL-CXTD-009), Qing Lan Project and NUPT 1311 projects for
their financial support.
Conflict of Interest
The authors declare no conflict of interest.
Keywords
charge trapping, filaments, photochromic memory, resistive switching
Received: October 7, 2016
Revised: April 30, 2017
Published online:
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