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Phosphorene—an emerging two-dimensional material: recent

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advances in synthesis, functionalization, and applications
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24 November 2021 Vivek Chaudhary1,2,∗, P Neugebauer3, O Mounkachi2,4, S Lahbabi2,5 and A El Fatimy1,3,∗
REVISED 1
19 April 2022 Institute of Applied Physics, Mohammed VI Polytechnic University, Lot 660, Hay Moulay Rachid, Ben Guerir 43150, Morocco
2
Modeling, Simulation and Data Analysis (MSDA), Mohammed VI Polytechnic University, Lot 660, Hay Moulay Rachid, Ben Guerir
ACCEPTED FOR PUBLICATION
43150, Morocco
6 May 2022 3
Central European Institute of Technology, CEITEC BUT, Brno University of Technology, Purkyňova 123, Brno 61200, Czech Republic
PUBLISHED 4
Laboratoire de Matière Condensée et Sciences Interdisciplinaires (LaMCScI), Faculty of Science, Mohammed V University in Rabat,
20 May 2022
Rabat 1014, Morocco
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Equipe Modélisation, Applications, Mathématiques et Informatiques (EMAMI), Laboratoire de Recherche en Ingénierie, ENSEM,
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Abstract
Two-dimensional (2D) materials are the focal point of intensive research efforts due to their
unique properties and ability to reveal fascinating new phenomena. As an analog to graphene,
phosphorene is a monolayer of black phosphorus crystals. Phosphorene obtained a special place
among the family of 2D semiconducting materials because of its fascinating features such as high
optical absorption, high carrier mobility, and several other attractive features having an exceptional
interest in electronic and optoelectronic applications. The anisotropic orthorhombic crystal
structure of phosphorene provides remarkable mechanical, electronic, optical, and transport
properties. This review summarizes phosphorene’s chemical and physical properties and highlights
the recent progress made in the synthesis. The application of phosphorene-based devices in
high-speed electronics and optoelectronics has been surveyed. Also, sufficient emphasis has been
given to emerging biomedical applications. Finally, phosphorene’s remaining challenges and
potential applications are outlined.

1. Introduction (h-BN) [11], MXenes [12, 13], carbon nitride [14],

The breakthrough discovery of graphene in 2004
has revolutionized the world of materials science.
Novoselov and Geim have successfully isolated a
monolayer of carbon atoms having hexagonal lat-
tice from graphite [1]. In 2010, this pioneering dis-
covery received Nobel Prize in Physics. Graphene
has extraordinary properties such as excellent elec-
trical conductivity, thermal conductivity, high trans-
parency, and high mechanical strength [2–4]. Since
its discovery, graphene has demonstrated excess-
ive promise in numerous applications in electron-
ics, photovoltaics, energy storage devices, and bio-
medical science [5–10]. The promising success of
graphene has instated a rapid surge in the quest
for two-dimensional (2D) materials. Several class
of 2D materials such as hexagonal boron nitride
transition metal oxides [15], elemental 2D materials
similar to graphene (i.e. germanene, silicene, stanene)
[16], and transition metal dichalcogenides (TMDs)
[17–28] have been discovered and developed as post
graphene 2D materials. These materials have gained
enormous attention due to their ubiquitous physical,
chemical, and electronic properties. Also, the ongoing
research activities on 2D materials have opened a new
avenue for developing post-silicon device techno-
logy. Among the family of 2D materials, molybdenum
disulfide (MoS2 ) is one of the most explored 2D
materials having a tunable bandgap from 1.8 eV for
monolayer to 1.2 eV for the bulk state [29]. Although
MoS2 provides a commendable ON/OFF ratio up
to 108 in resulting devices and amends the zero-
bandgap weakness of graphene, it suffers from the low
charge carrier mobility compared to graphene [30].

© 2022 The Author(s). Published by IOP Publishing Ltd

2D Mater. 9 (2022) 032001
Figure 1. Representation of various allotropic forms of the phosphorous.
The bandgap of a semiconductor material plays a
crucial role in the overall performance of field-effect
transistors (FETs) devices. The high ON/OFF ratio is
a prerequisite for exploiting FETs in digital logic cir-
cuits. The On-state current does not directly depend
on the bandgap (Eg ). However, the OFF-state current
is governed by thermionic emission of charge carri-
ers through the metal/semiconductor Schottky bar-
rier. Therefore, the OFF-state current is proportional
to exp (−eφB /kb T), where e is the electronic charge,
φB is Schottky barrier height, kb is the Boltzmann
constant, and T is the temperature. Further, consider-
ing the work functions of metal contact and semicon-
ductor,(the OFF-state
) current would be proportional
to exp −Eg /nkb T , where n is related to the differ-
ence between work functions of metal and semicon-
ductor.
( This makes
) the ON/OFF ratio proportional to
exp Eg /nkb T [31]. Thus, for the lowest acceptable
on/off ratio, i.e. up to three to four orders of mag-
nitude at room temperature, the bandgap should be
at least 0.4 eV for digital logic applications.
Therefore, an ideal 2D material should have high
charge mobility and a suitable bandgap. In recent
years, black phosphorus (BP) has acquired a niche in
the elemental 2D materials family and can bridge the
gap between graphene and TMDs. Phosphorus is one
of the most abundant elements in the Earth’s crust,
occupying about 0.1% volume. Phosphorus mainly
exists in the form of four allotropes, namely white
phosphorus (WP), red phosphorus (RP), violet phos-
phorus (VP), and BP. Figure 1 expresses different
allotropic phases of phosphorous. WP is composed of
four phosphorous atoms forming a cubic lattice and
is extremely unstable under ambient conditions. RP
is an amorphous network of phosphorous atoms con-
nected via covalent bonds, whereas VP is constituted
in monoclinic structure. Among all the allotropes of
2
V Chaudhary et al
phosphorus, BP is harmless and exhibits the highest
structural and thermodynamic stability. BP is one of
the fascinating allotropes of phosphorous having an
orthorhombic crystal structure and was first synthes-
ized by Bridgman [32]. After its discovery, BP has
received very marginal research interest almost for
a century. It has gained a blooming consideration
since 2014 when the monolayer of BP named ‘phos-
phorene’ was successfully exfoliated by two independ-
ent research groups [33, 34]. Phosphorene was first
exfoliated from bulk BP crystal via the scotch-tape
microcleavage method [33]. The most exciting prop-
erty of BP includes (a) layer dependent bandgap ran-
ging from 0.3 eV for bulk to 2.0 eV for monolayer
[35, 36], (b) unlike other TMDs 2D materials, BP
nanosheets always have direct band structure for any
number of layers [35, 37], (c) BP nanosheets demon-
strate a high degree of in-plane anisotropy resulting in
angle-dependent optical and electrical conductivity
[38]. In addition, it has been reported that few-layer
phosphorene (thickness 10 nm) assimilated remark-
able field-effect mobility of 1000 cm2 V−1 s−1 and
drain current modulation up to 105 at room temper-
ature, which is much higher than 2D TMDs while
less than graphene [34]. Also, the quantum Hall effect
has been observed on few-layer phosphorene samples
with Hall mobility approaching 6000 cm2 V−1 s−1 at
temperatures below 30 K [39]. Apart from highly
tunable direct bandgap, high charge carrier mobil-
ity, and in-plane anisotropy, few-layer phosphorene
has other distinctive features such as nominal electric
resistance, excellent mechanical strength, large sur-
face area, and high thermal stability. These remark-
able properties explain that BP or few-layer phos-
phorene can be employed as an eligible candidate in
various electronic devices like FETs, photodetectors,
solar cells, terahertz imaging, batteries, etc [40–52].
2D Mater. 9 (2022) 032001
Although recent studies and research suggest sev-
eral feasible advantages of phosphorene, the success-
ful experimental demonstration of phosphorene at
the device scale is still limited due to synthesis and
stability challenges.
The development of BP and phosphorene has
been systematically and comprehensively demon-
strated in the present review. A general overview of BP
and phosphorene’s properties with their benefits and
a detailed study on the synthesis methods currently
being used and their challenges are presented. This
review outlines the progress achieved so far in various
areas of science and technology through the applica-
tion of phosphorene or BP. Based on the suitability
of atomic structure and elemental properties, phos-
phorene and its derivatives employed in emerging
electrical devices such as solar cells, FETs, sensors, and
biomedical applications have been explored. Finally,
discussing the current challenges in phosphorene syn-
thesis, the review elucidates critical future directions
for high-quality phosphorene synthesis and its applic-
ations in various science and technology regimes.
2. Structure and fundamental properties
BP crystals appear black and flaky, just like graph-
ite, as shown in figure 2(a). BP has a layered struc-
ture analogous to graphite. The layered structure
of multilayer BP in the AB-stacking pattern has
been demonstrated in figure 2(b). The interlayer dis-
tance between the consecutive stacked layers of BP
is 5.3 Å [53, 54]. The distance between the lay-
ers in BP is significantly greater than the length of
the P–P covalent bonds (∼2.2 Å) [55], which indic-
ates that the BP layers are packed together through
a non-bonding van der Waals interaction. Further,
the cohesive energy of BP layers is found to be
∼20 meV atom−1 [33], resembling that of graphite
and hBN (∼30 meV atom−1 ) [56, 57].
The structure of BP was first studied by Hultgren
et al [58] and further modified by Brown et al [59].
The high structural stability of BP arises from its
orthorhombic crystalline structure and contains eight
atoms per unit cell. In BP, phosphorus (P) atoms have
sp3 hybridization, and each P atom forms covalent
bonds with three adjacent atoms, out of which two
lie on the same plane while the third one lies on the
neighboring plane with one-electron pair [60]. This
hybridization gives rise to a quadrangular pyramid
structure analogous to puckered honeycomb-like
structure, and consequently, the asymmetric band
structure evolves with peculiar anisotropic proper-
ties [61, 62]. The top and side view of monolayer
phosphorene is illustrated in figure 2(c), where the
atom in different colors demonstrates atoms located
in different planes. It is evident from figure 2(c) that
phosphorene exhibits a puckered structure relative to
the armchair direction but looks like a bilayer atomic
3
V Chaudhary et al
configuration when viewed relative to the zigzag dir-
ection. The folded structure of phosphorene maxim-
izes the separation between electron pairs of each P
atom located in either plane, reducing the degree of
orbital hybridization.
The dotted lines in figure 2(c) represent a unit
cell of monolayer phosphorene. It has been found
that phosphorene has different lattice constants along
the two perpendicular directions. Also, the lat-
tice constant varies as: a = 4.52 ± 0.05 Å and
b = 3.31 ± 0.03 Å (the directions of ‘a’ and ‘b’ are
depicted in figure 2(c)) with respect to the number of
layers [33, 38, 63, 64]. It should be noted that bulk
BP and phosphorene have the same in-plane sym-
metry with the base-centered orthorhombic struc-
ture. Based on the first principle calculations by Qiao
et al [38], the lattice parameter ‘a’ increases from
4.47 Å (bulk BP) to 4.58 Å (monolayer phosphorene),
whereas the lattice parameter ‘b’ decreases from
3.34 Å (bulk BP) to 3.32 Å (monolayer phosphorene).
Moreover, two different bond angles/lengths exist
concerning in-plane and out-plane atomic arrange-
ment, as illustrated in figure 2(d). The angle between
P atoms on the same plane is designated as θ2 (hinge
angle), while the angle between atoms on different
planes is represented as θ1 (dihedral angle). A slight
effect of layer number is observed on the dihedral (θ1 )
and hinge (θ2 ) angles. The dihedral/hinge angles vary
from 102.42◦ /96.16◦ to 103.51◦ /96.00◦ , respectively
for bulk BP and monolayer phosphorene [38]. In the
same analogy, the bond lengths between P atoms on
the same plane are defined as R2 and those on differ-
ent planes as R1 . However, it has been observed that
there is no prominent effect of the layer number on
the bond length. Two of the three nearest P atoms
lying in the same plane have a bond length of 2.224 Å
(R2 ), whereas the third P atom lying out of the plane
has a bond length of 2.244 Å (R1 ) [55].
As a semiconductor, phosphorene is a promising
material due to its extraordinary physical and chem-
ical properties, as depicted in table 1. In comparison
to other 2D layered materials, phosphorene demon-
strates the enormous potential for several applica-
tions. The physical properties of phosphorene and
other most explored 2D materials such as graphene,
MoS2 , WSe2 , and h-BN have been compared (table 1)
to establish their importance. It can be concluded
from table 1 that phosphorene does not exhibit the
best values for all the physical quantities, but it equi-
librates the properties of the 2D family.
For example, the forefather graphene exhibits
the highest carrier mobility (∼105 cm2 V−1 s−1 ),
thermal conductivity, and mechanical strength; how-
ever, it suffers from a meager ON/OFF ratio due
to zero bandgap. On the contrary, MoS2 and WSe2
demonstrate a very high ON/OFF ratio because of
their band structure and have good applicability
in thermoelectric devices. However, these materials’
2D Mater. 9 (2022) 032001 V Chaudhary et al

Figure 2. (a) Image of bulk BP crystal. Reproduced with permission from smart-elements.com. (b) Perspective side view of
multilayer BP (c) top and side view of monolayer phosphorene. ‘a’ and ‘b’ represents the lattice parameters. (d) Representation of
structural arrangement of the atoms illustrating dihedral/hinge angles and bond lengths. The different color of P atoms in each
figure represents the P atoms located in different planes.

Table 1. Comparison of fundamental properties of various 2D materials.

Parameters Graphene MoS2 WSe2 h-BN Phosphorene

Nature Semimetal Semiconductor Semiconductor Insulator Semiconductor

Bandgap (eV) 0 1.2–1.8 1.2–1.7 5.9 0.3–2.0
Carrier type Ambipolar n-type Ambipolar — Ambipolar
Mobility 2 × 105 10–200 150–500 — 103
(cm2 V−1 s−1 )
ON/OFF ratio 5–50 106 –108 104 –106 — 103 –105
Thermal 5 × 103 34–52 10 250–360 10–36
conductance
(W m−1 K−1 )
Young’s modulus 103 270–400 75–200 200–900 35–166
(GPa)
References [3, 65–71] [65, 72–78] [65, 72, 79–85] [65, 86–88] [33, 34, 89–92]

substandard charge transport and carrier mobil-
ity limit their widespread applications in several
fields. Further, h-BN provides a versatile platform for
research and advancement in water electrolysis, fuel
cells, etc. Also, the electrically insulating behavior of
h-BN makes it a potential candidate as encapsula-
tion and gate dielectric material. Undoubtedly, 2D
phosphorene provides many intriguing optical and
electronic properties such as non-equilibrium band
broadening, bandgap inversion and renormalization,
electronic work function modulation, and intentional
defect formation as well as their anisotropic migra-
tion, which are very beneficial for (Opto)electronic
device applications [93–97].
The material’s energy bandgap plays a crucial role
in device applications, particularly in optical sensors

4
2D Mater. 9 (2022) 032001 V Chaudhary et al

Figure 3. (a) Variation of the bandgap of phosphorene with the number of layers calculated by different theoretical and
experimental methods. Reprinted figure with permission from [36], Copyright (2014) by the American Physical Society. (b) The
bandgap values of conventional and 2D layered semiconductors with their maximum variation range. The bottom of the figure
shows various possible applications depending on the bandgap. Reprinted with permission from [101]. Copyright (2015)
American Chemical Society.

and solar cells [98, 99]. Phosphorene offers a highly
tunable bandgap ranging from 0.3 to 2.0 eV depend-
ing on the number of layers and stacking pattern, as
depicted in figure 3(a). The bandgap range of phos-
phorene is remarkably higher than that of graphene
and almost similar to that of layered 2D chalco-
genides, making phosphorene an ideal material for
diverse applications [33, 34, 63, 100]. Apart from
highly tunable bandgap, phosphorene exhibits direct
band nature for all thicknesses, which attracts great
interest because other 2D layered semiconductors
possess indirect band structure in their multiple lay-
ers [35, 37]. Gomez et al [101] established the exclus-
iveness of phosphorene by comparing the bandgap
value of various 2D layered and compound semicon-
ductors. Figure 3(b) demonstrates the highest degree
of bandgap tunability of phosphorene in comparison
with other 2D materials, which provides the possibil-
ity to achieve the desired bandgap value that is essen-
tial for a particular application. Due to this unique
bandgap structure, phosphorene can be considered a
suitable candidate for potential use in various applic-
ations, as depicted at the bottom of figure 3(b).
The recent studies on phosphorene and bulk
BP reveal that phosphorene exhibit a high degree
of anisotropy in optical absorption. Since the crys-
tal structure of phosphorene possesses an inver-
sion symmetry and mirror reflection symmetry only
along the zigzag direction, the anisotropy in the
optical absorption of phosphorene emerges from the
symmetry-forbidden selection rule. Therefore, the
phosphorene exhibits linear dichroism, i.e. the optical
absorption properties of phosphorene vary with the
change of direction, showing different properties in
different directions (armchair and zigzag) and also
depend on the state of polarization of incident light.
Qiao et al [38] studied the absorption behavior of
differently polarized light in phosphorene and bulk
BP and concluded that the absorption energy edges
decrease with increasing the number of layers in
both armchair and zigzag directions. However, the
decreasing rate in the armchair direction is much
higher than that in the zigzag direction. Ling et al
[102] established that the light polarized in the arm-
chair direction was more easily absorbed than that
in the zigzag direction. Figure 4(a) demonstrates the
calculated coefficient of optical absorption (α) for
zigzag and armchair polarized light with respect to
layer thickness. The variation of α with incident
energy reveals that the absorption starts at much
lower energy for the armchair polarized light in com-
parison to that of zigzag polarized light. Also, there is
no significant effect of the layer numbers on the α for
the same polarized light, indicating that absorbance
should be increased with increasing thickness.
Further, the measured optical absorption spec-
tra of a thin and thick BP sheet for armchair and
zigzag polarized light are presented in figure 3(b),

5
2D Mater. 9 (2022) 032001 V Chaudhary et al

Figure 4. (a) Variation of absorption coefficient in mono/bi/tri/ten-layer phosphorene and bulk BP with respect to laser energy.
(b) Typical optical absorption spectra of thin and thick BP nanosheets with incident light polarized along with armchair and
zigzag directions. Reprinted with permission from [102]. Copyright (2016) American Chemical Society.

which manifest a similar anisotropic behavior to the
calculated one. Furthermore, He et al [103] repor-
ted that armchair direction possesses 16 times higher
photon diffusion efficiency and ten times more signi-
ficant absorption coefficient than that in zigzag direc-
tion. The anisotropic structure of phosphorene also
demonstrates crystal orientation-dependent charge
carrier recombination. It is reported in the literat-
ure that the exciton wave function of monolayer
phosphorene exhibits direction-dependent probabil-
ity density [36, 104]. The probability density of the
exciton wave function is much more dispersed in
the armchair direction than that in the zigzag dir-
ection. The photoluminescence spectra of monolayer
phosphorene exhibit enhanced emission when recor-
ded in armchair direction, i.e. the emission from
phosphorene is highly dependent on the induced
polarization. The phosphorene shows photolumines-
cence emission with the highest intensity when the
excitation and detection polarization is in the arm-
chair direction, while at the same time, the emis-
sion intensity in the zigzag direction is only 3%
of that in the armchair direction [104, 105]. Also,
the electron–photon interaction becomes more pro-
nounced for the incident light polarized in the arm-
chair direction. Due to its unique anisotropic optical
properties and wide absorption range, phosphorene
holds a promising application in (opto)electronics,
linear/nonlinear optics, and photocatalysis.
Electrical conductivity is one of the essential para-
meters to determine the quality of semiconductors.
Bridgman first studied the electrical conductivity of
BP in 1921. The early studies demonstrated that the
resistivity of BP ranges from 0.48 to 0.77 Ω cm at
room temperature [106]. The high carrier mobility is
an outstanding inherent property of bulk or few-layer
BP, which has attracted the attention of researchers
to this new material. Recently, massive efforts have
been made to develop practical applications of this
material. Like optical properties, phosphorene exhib-
its anisotropy in electrical transport also. Since charge
mobility is a function of the effective mass of the
charge carriers, the effective mass of charge carriers
in phosphorene is found to be direction-dependent.

6
2D Mater. 9 (2022) 032001
Figure 5. (a) Variation of electron effective mass with respect to spatial direction pristine phosphorene and (b) after applying 5%
biaxial strain. Reprinted with permission from [91]. Copyright (2014) American Chemical Society. (c) Variation in DC
conductivity (solid dots) and polarization-resolved relative extinction coefficient (hollow squares) along six different directions
separated by 30◦ on the same phosphorene sheet. Inset shows an optical image of the phosphorene sheet. Reproduced from [100],
with permission from Springer Nature.
Due to phosphorene’s orthorhombic puckered struc-
ture, the effective mass of charge carriers has been
found to be ten times lesser in armchair direction
than that in the zigzag direction, which justifies that
the armchair direction is much more favorable for
charge transport [54].
Fei et al [91] established that strain engineer-
ing could also significantly tune the electrical con-
duction of phosphorene. Under the application of
suitable uniaxial/biaxial strain on phosphorene, the
anisotropy of effective mass of the electrons and
their mobility can be rotated to 90◦ as described
in figures 5(a) and (b). Also, the effective mass of
electrons in the zigzag direction decreases signific-
antly and abruptly increases in the armchair direc-
tion, notifying that the zigzag direction offers favor-
able electron transport in this case. However, the
anisotropy of the effective mass of holes remains
unchanged for any applied stress or strain. The angle-
resolved DC conductivity measurements on phos-
phorene nanosheets are presented in figure 5(c). The
results very nicely demonstrate the direction depend-
ence of electrical conductivity/mobility in the phos-
phorene layer. Further, the ratio of charge mobility in
two different directions has been observed to be 1.5
[100]. The phosphorene’s highly anisotropic charge
transport features imply a big room for further under-
standing and development of practical applications
where the anisotropic charge transport is desired.
3. Synthesis routes and challenges
Generally, the synthesis of atomically thin 2D nan-
omaterials can broadly be divided into two meth-
ods, namely the ‘top-down method’ and the ‘bottom-
up method’. It has been well established that 2D
layered materials are bonded by weak interplanar
van der Waals force and strong in-plane covalent
bonding. For example, graphite is a distinguished
class of materials composed of weakly stacked planer
graphene sheets [107]. Analogous to graphite, BP
7
V Chaudhary et al
is also a layered material having individual atomic
sheets bonded together by weakly interacting van
der Waals force. In BP, the interlayer stacking dis-
tance depends on the stacking pattern and is found
to be ∼5.3 Å, as demonstrated in figure 2(b) [53, 54].
The range and pattern of interlayer stacking of indi-
vidual layers on BP crystals provide a possibility
to obtain atomically thin phosphorene sheets util-
izing simple top-down exfoliation techniques. On
the contrary, the bottom-up methods such as wet
chemical synthesis and chemical vapor deposition
(CVD), etc, result in the direct growth of materials via
chemical reactions.
3.1. Top-down routes
The top-down route for nanomaterials synthesis
involves breaking bulk material into nanoscale struc-
tures or particles. It follows an inherently straight-
forward mechanism of removal or division of bulk
material to their respective nanometer-sized atomic
configuration. However, the top-down route offers a
facile preparation process for the phosphorene and
other 2D materials but lacks precise control on the
lateral dimension and layer number in the obtained
structures/thin films. Inspired from the mechanical
exfoliation of graphite to graphene sheets, a similar
sticky-tape microcleavage analogy has been employed
on BP crystal to obtain mono/few-layer nanosheets of
BP. It has been established from the quantum chem-
ical simulations that the energy for BP exfoliation is
approximately 151 meV atom−1 [108]. This amount
of exfoliation energy infers that BP can be peeled off
to its mono/few-layer nanostructures via the applic-
ation of different driving forces. For the first time in
2014, Liu et al [33] demonstrated the exfoliation of BP
crystal via mechanical cleavage and obtained atom-
ically thin mono/few-layer phosphorene over SiO2 /Si
substrate. At the same time, Zhang et al [34] reported
the mechanical exfoliation of BP down to 10 nm using
sticky-tape method. The mechanical cleavage tech-
nique has produced high-quality 2D phosphorene
2D Mater. 9 (2022) 032001
Figure 6. Schematic growth of phosphorene sheet via metal-assisted exfoliation. Reproduced from [112] with permission from
the Royal Society of Chemistry.
sheets, but the yield was poor. Also, the contamina-
tion in the form of adhesive residue over the phos-
phorene surface hinders its practical application. Fur-
ther, the shape, size, and thickness of the resulting 2D
nanosheets could not be controlled via the mechan-
ical cleavage method. Since the most important and
peculiar features of 2D phosphorene depend on the
layer thickness, the focus has been shifted to alternat-
ive ways that can produce high-quality phosphorene
sheets with control over the layer thickness.
In this quest, Gomez et al [109, 110] modified
the traditional exfoliation technique using an inter-
mediate viscoelastic polydimethylsiloxane surface to
peel off the phosphorene layer from the bulk BP crys-
tal. This technique significantly increased the pro-
duction yield of the phosphorene sheet, and the
obtained layers were free from chemical contamina-
tion of adhesive traces. Lu et al [111] introduced the
combination of traditional mechanical cleavage fol-
lowed by the Ar+ plasma thinning process and could
achieve stable phosphorene sheets ranging from 1 to
5 layers. Furthermore, Gaun et al [112] reported a
metal-assisted mechanical cleavage method to peel
off phosphorene sheets. In their work, the authors
used a few nm metals (Au/Ag) deposited substrates
(SiO2 /Si) and pasted a blue tape with BP onto the
substrate, followed by heating. After that, the blue
tape was torn off from the substrate, followed by
metal layer etching. The schematics of metal-assisted
mechanical cleavage method are presented in figure 6.
This technique could produce phosphorene layers
with a grain size of more than 50 µm. Although
8
V Chaudhary et al
mechanical cleavage has been proven to be an effect-
ive method to get mono/few layers of phosphorene
with larger domain size, the degradation of mechan-
ically cleaved phosphorene under an ambient envir-
onment is a severe drawback. Despite these restric-
tions, considerable efforts have been made to prepare
phosphorene via mechanical exfoliation to explore
the possible applications and study the degradation
mechanism [100, 113–121].
Liquid exfoliation is another versatile technique
that is being extensively used to produce atomically
thin 2D nanosheets of layered materials [122, 123].
In this technique, the final materials are produced
in liquid dispersions with a large amount of 2D
nanosheets. The liquid phase exfoliation is an inter-
esting method for 2D materials flake exfoliation
and is compatible with the requirement of indus-
trial production. In liquid exfoliation, ultrasound
waves create microscopic bubbles in the liquid, and
the average size of bubbles can be optimized with
the ultrasound waves’ frequency and power. These
microscopic bubbles contract at a high-pressure cycle,
expand at low pressure, and further explode violently
during the pressure change, leading to the cavitation
effect [122]. The cavitation effect instantaneously
generates a very high pressure of more than 100 MPa
within a hotspot. The continuous explosion of these
microscopic bubbles near the surface of 2D materi-
als exerts shear force by forming microjets that punch
on the surface. The sheer force and microjet punch-
ing on the surface of 2D materials weakens the van
der Waals force and promotes the separation of layers,
2D Mater. 9 (2022) 032001 V Chaudhary et al

Figure 7. (a) Schematics of liquid exfoliation of BP into phosphorene nanosheets in N-methyl-2-pyrrolidone (NMP) assisted by
NaOH and corresponding AFM image of obtained nanosheets. [124]. John Wiley & Sons. Copyright (2015) WILEY-VCH Verlag
GmbH & Co. KGaA, Weinheim. (b) Liquid exfoliation of BP in ionic liquid and corresponding AFM image of obtained
nanosheets. Reprinted with permission from [125]. Copyright (2015) American Chemical Society. (c) Schematics of solvothermal
assisted liquid exfoliation of BP in acetonitrile and corresponding AFM image of obtained nanosheets. Reprinted from [126],
Copyright (2018) The Chinese Ceramic Society. Production and hosting by Elsevier B.V.

causing the exfoliation of material to mono or few lay-
ers. The liquid exfoliation technique provides several
advantages, such as the possibility of thin-film forma-
tion over any substrate from rigid to flexible, produc-
tion of composite/hybrid materials, and feasibility of
the roll-to-roll fabrication process. In general, liquid
exfoliation is based on ion exchange/intercalation or
surface passivation by the solvent molecules and pro-
duces a very high yield of 2D nanosheets with a
straightforward and cost-effective approach.
Brent et al [127] were the first to report the liquid
exfoliation of BP down to three-to-five-layer phos-
phorene with a lateral size of 200 nm via bath ultra-
sonication of BP in N-methyl-2-pyrrolidone (NMP)
for 24 h. It has been observed that BP can be effi-
ciently exfoliated into mono/bilayer phosphorene by
prolonged ultrasonication (up to 48 h); however, it
significantly reduces the lateral flake size to 20 nm.
Yasaei et al [128] reported the exfoliation of BP
in dimethyl sulfoxide and dimethylformamide. The
inert and polar nature of the solvents produced
highly dispersed atomically thin phosphorene sheets
in the suspensions. Also, the obtained phosphorene
sheets were resistant to degradation and demon-
strated remarkable electrical properties compared to
mechanically exfoliated BP. Hanlon et al [129] exfoli-
ated BP in N-cyclohexyl-2-pyrrolidone and obtained
high-grade few-layer phosphorene with control over
size distribution and enhanced photoluminescence.
The phosphorene sheets thus obtained were enclosed
with a solvation shell which avoided corrosion caused
by oxygen or moisture. Guo et al [124] introduced
the NMP/NaOH mixture as an excellent solvent and
obtained a high phosphorene dispersion yield down
to ∼5 layers, as shown in figure 7(a). The phos-
phorene nanosheets thus obtained were stable even
in water.
Besides liquid solvents, Zhao et al [125] used
the ionic liquid to prepare a highly concentrated
and stable dispersion of phosphorene. Figure 7(b)
demonstrates the schematics of BP exfoliation in
ionic liquid. The exfoliation of BP in ionic liquid
resulted in phosphorene layer thickness down to
3.58 nm, as evident from the atomic force microscopy

9
2D Mater. 9 (2022) 032001
(AFM) image (figure 7(b)). The prepared phos-
phorene dispersion was stable under the ambient con-
ditions for almost 30 d without any noticeable aggreg-
ation or sedimentation. The solvothermal-assisted
liquid-phase exfoliation in the presence of acetonitrile
was proposed by Yan et al [126] to obtain very thin
(∼2 nm) phosphorene sheets (figure 7(c)) with a lat-
eral size of more than 10 µm. In this method, bulk
BP and acetonitrile were mixed in an autoclave and
subjected to heating at 200 ◦ C for 24 h. The obtained
product was subjected to ultrasonication followed by
centrifugation to get the phosphorene layers. Very
recently, Watts et al [130] reported the formation
of phosphorene nanoribbons via Li-ion intercalation
followed by ultrasonication in NMP. The dimen-
sion of obtained ribbons was 690 nm in length and
30 nm in width. Many other researchers have synthes-
ized stable phosphorene dispersion following liquid
phase exfoliation [131–144]. The liquid phase exfo-
liation technique provides a facile and environment-
ally friendly way to obtain mono to few-layer phos-
phorene, which is desired to study the fundamental
properties and practical applications of this novel
material.
3.2. Bottom-up routes
The bottom-up route is traditional to produce ultra-
thin sheets of 2D materials via chemical reactions.
In general, the wet chemical self-assembly methods
and CVD method are the most reliable bottom-up
techniques for the large-scale synthesis of nanoma-
terials [145, 146]. The bottom-up method involves
the synthesis of nanostructures by stacking atoms or
molecules onto each other, which forms nanoclusters
of atoms or molecules on the substrate. Further, these
nanoclusters stack on each other, resulting in a uni-
form thin film on the substrate. Also, the bottom-up
method offers very precise control on the thickness
and lateral size of the resulting thin film or nanostruc-
tures. Although wet chemical methods such as sol-
vothermal, hydrothermal, and template-assisted self-
assembly/growth have resulted in mass production of
graphene, TMDs, and other 2D materials, the pres-
ence of high pressure, moisture, and oxygen in these
methods imposes severe limitations on the growth of
phosphorene. However, the oxygen-free environment
such as boiling water and or organic solvents may lead
to the successful synthesis of phosphorene with these
methods. In this approach, Zhang et al [147] success-
fully synthesized phosphorene composite nanosheets
via wet chemical synthesis using RP as starting pre-
cursor. The lateral dimension of obtained nanosheets
was around 1.0 µm with thickness ranging from 0.5
to 4 nm. Zhao et al [148] further modified this tech-
nique by adding ammonium fluoride to the precursor
mixture, followed by heating at 200 ◦ C for 16 h in
an autoclave. This synthesis protocol resulted in the
formation of bilayer phosphorene sheets that were
capable of efficiently separating the photoinduced
10
V Chaudhary et al
charge carriers and showed high photostability. Tian
et al proposed another facile approach for syn-
thesizing few-layer phosphorene nanosheets via wet
chemical method using WP and ethylenediamine
[149, 150]. These wet-chemical methods of produ-
cing phosphorene exhibit the potential for scalable
production with multiple perspectives such as uni-
form size, controllable thickness, and high through-
put, which is essential for successful application.
Besides wet-chemical routes for the bottom-up
synthesis of 2D materials, CVD offered a grand prom-
ise in the high-quality, large-scale production of
monolayer graphene, TMDs, and other elemental 2D
materials. The challenges such as the lack of adequate
substrate and precursors restrict the large-scale CVD
growth of phosphorene. However, a few approaches,
which are almost identical to CVD, should be dis-
cussed in order to improve the synthesis methods and
the quality of phosphorene. Li et al [153] were the first
to propose the CVD-like synthesis of BP thin film on
a flexible substrate. They started with RP powder and
deposited it on a flexible substrate at 400 ◦ C using
thermal evaporation. After growth, it was subjected
to a multi-anvil cell at a pressure of 10 GPa to con-
vert the RP into BP. Thus obtained BP film was found
to have a thickness of 40 nm. Further, Smith et al
[154] synthesized few-layer phosphorene with an area
ranging from 0.35 to 100 µm2 . In the typical pro-
cess, the RP was first deposited on SiO2 /Si substrate
at 600 ◦ C via thermal evaporation in a tube furnace
under vacuum conditions. After the growth of homo-
genous RP thin film, it was placed in a centrifuge tube
with Sn and SnI4 mineralizing agents, and then the
whole system was placed in a pressure vessel reactor
filled with argon (27.2 atm) followed by heating at
900 ◦ C. Very recently, Xu et al [151] reported growth
of highly crystalline few-layer phosphorene on Au
coated SiO2 /Si substrate. The key idea was to use the
intermediate polyphosphate species (Au3 SnP7 ) as a
nucleating layer for further growth of phosphorene. It
is evident from figure 8(a) that this method demon-
strated excellent scalability over the lateral size (a
few microns to sub-millimeters) and precise control
over the thickness (few nm to hundreds of nm) of
produced nanosheets.
In the scenario of a bottom-up approach, other
methods like molecular beam epitaxy and pulsed
laser deposition have also been employed to grow
phosphorene nanosheets [155]. Wu et al [152] fab-
ricated ultra-thin phosphorene sheets on mica sub-
strate via pulsed laser deposition. They started with
bulk BP crystal as the source materials and freshly
exfoliated mica wafer as substrate and obtained
centimeter-scale few-layer phosphorene under ultra-
high vacuum conditions (see figure 8(b)). Also, it has
been observed that the layer number in the result-
ant films can be precisely controlled by varying the
number of laser pulses during the growth process.
These sequential studies on the bottom-up approach
2D Mater. 9 (2022) 032001 V Chaudhary et al

Figure 8. (a) (i) Schematic view of controlled growth of few-layer phosphorene nanosheets on Au coated SiO2 /Si substrate.
((ii)–(v)) The optical (top) and corresponding AFM (bottom) images of phosphorene nanosheets with their lateral size (several
microns to few millimeters) and thickness (few nm to hundred’s of nm) under controlled growth conditions. Reproduced from
[151]. CC BY 4.0. (b) (i) Schematics of controlled growth of phosphorene via pulsed laser deposition technique. AFM images of
(ii) monolayer phosphorene (iii) bilayer phosphorene. Reproduced from [152], with permission from Springer Nature.

of phosphorene synthesis pave the way to develop BP-
based wafer-scale devices with potential applications.
4. Functionalization and stability
In general, 2D materials are functionalized to tune the
physical and chemical properties that match a partic-
ular application’s desired features. For phosphorene,
functionalization is required to prevent the degrada-
tion caused by moisture, oxygen, and light. The lone
pair of electrons in phosphorene reacts with atmo-
spheric oxygen forming Px Oy , and the exposure of
light increases the rate of this reaction [156, 157].
The degradation mechanism of phosphorene is not
yet well understood and is currently being systemat-
ically investigated. Many functionalization methods
are presently being used to enhance the stability of
phosphorene. The strategies such as encapsulation,
passivation using non-covalent interaction, forma-
tion of heterostructure with other 2D materials, and
introduction of a thin oxidized protecting layer are
essential in stabilizing phosphorene thin films [158].
Diverse results are obtained based on the interaction
between phosphorene and the protective layer, for
example, covalent or non-covalent. Such as, the cova-
lent type of interaction between phosphorene and the
protective layer could alter the intrinsic properties,
whereas the non-covalent type of interaction provides
an advantage of preventing fundamental properties.
The functionalization of phosphorene is particularly
appealing in view of synthesizing heterojunctions for
optoelectronic, photonic, chemical sensing, and bat-
tery applications [159, 160].
Gusmao et al [161] demonstrated the function-
alization of exfoliated phosphorene nanosheets using
redox probe anthraquinone. To obtain protective cap-
ping over phosphorene nanosheets, it was redispersed
with anthraquinone in methanol. The coating of
anthraquinone over phosphorene not only prevents
it from degradation but also provides enhanced elec-
troactive functionality. Liang et al [162] applied hexa-
methylenediamine self-assembled monolayer coating
over phosphorene, maintaining its elemental form
in the solution for more than 1 month. Further, an
effortless and straightforward non-covalent encapsu-
lation technique of phosphorene using helical poly-
mers was proposed by Kumar et al [163]. This pas-
sivation method is of particular importance since it
preserves the inherent intrinsic properties of phos-
phorene. The functionalization of phosphorene with
organoboron derivatives of a conjugated fluores-
cent molecule (pyrene) resulted in tremendous sta-
bility for more than 6 months with the electronic
structure modification at phosphorene/conjugated
organic molecule through non-covalent stabilizing
interactions mediated by boron atoms [164].
The functionalization of phosphorene with metal
nanoparticles (NPs) resulted in exotic properties and
has shown various potential applications in electronic
devices, catalysis, and the biomedical field. Several
research groups functionalized the phosphorene sur-
face with Au NPs and documented enhanced per-
formance for optoelectronic devices, photocatalysis,
and cancer/tumor therapy [165–168]. The loading
of Pt NPs on phosphorene nanosheets demonstrated
excellent hydrogen sensing and attractive applicabil-
ity in photodynamic anticancer therapy [169–173].
The impact of functionalization of phosphorene with
metal NPs in the sensing and biomedical field has
been thoroughly discussed in the application section
of this review.

11
2D Mater. 9 (2022) 032001
5. Applications
Although research on phosphorene began in 2014,
this novel 2D material has achieved promising suc-
cess. The synthesis techniques available in the present
and excellent properties of phosphorene demon-
strated potential applications in several fields of mod-
ern technology. In this section, various device applic-
ations of phosphorene, such as transistors, sensors,
and photodetectors, have been demonstrated. In
addition to electronic and optoelectronic applica-
tions, the importance of phosphorene has also been
shown in drug delivery and biomedical applications.
Also, the time-to-time advancement that has been
made to further improve phosphorene technology
is discussed.
5.1. Electronic devices
As an application to electronic devices, few-layer
phosphorene was first used as a channel material
in FETs by Li et al [33]. In this work, a mech-
anically exfoliated phosphorene sheet of thickness
below 10 nm was used to fabricate FETs, which
demonstrated an ON/OFF ratio as high as 105
with mobility 1000 cm2 V−1 s−1 at room temperat-
ure (figure 9(a)). After the first successful demon-
stration of few-layer phosphorene in FETs, many
research groups started to explore the device applic-
ations of this novel material [33, 100, 109, 120, 121].
Although few-layer phosphorene has proven itself as
a high-performing semiconductor material in FETs,
its devices exhibit significant fluctuations in current
due to the trapping/detrapping of charge carriers at
the interface. Na et al [174] applied a very thin Al2 O3
layer over the fabricated few-layer phosphorene FET
devices to rectify this issue. The transport charac-
teristics of both bare and passivated few-layer phos-
phorene FETs were studied using static and low-
frequency noise analyses. The results demonstrated
that after passivation with Al2 O3 , the noise level of the
drain current was drastically decreased over the whole
operating region, as depicted in figures 9(b) and (c).
Apart from reducing noise levels and current fluc-
tuations, the Al2 O3 passivation layer also improves
the device’s stability against atmospheric degrada-
tion. To establish this fact and understand the rela-
tionship between few-layer phosphorene and Al2 O3 ,
Wood et al [120] studied the performance of few-layer
phosphorene FETs with and without AlOx passivation
layer concerning aging time. It has been observed that
bare few-layer phosphorene FETs show a significant
increase in threshold voltage followed by a 103 times
decrease in ON/OFF ratio within 6 h after atmo-
spheric exposure and the carrier mobility goes down
to 10−2 cm2 V−1 s−1 within 50 h (figure 9(d)). How-
ever, the FETs encapsulated with AlOx layer are found
to maintain their performance for up to 2 weeks with
mobility approaching 100 cm2 V−1 s−1 .
12
V Chaudhary et al
Xu et al [151] recently realized a few-layer
phosphorene-based FETs via a gas-phase growth
approach having layer thickness ∼5–10 nm. The fab-
ricated FET devices demonstrated Hall and field-
effect mobility over 1400 and 1000 cm2 V−1 s−1
at room temperature, respectively, as depicted in
figures 9(e) and (f). The array of 25 FETs on a
5 nm thin centimeter-scale phosphorene layer has
been fabricated by Wu et al [152]. The fabricated
devices yielded field-effect mobility up to 213 and
617 cm2 V−1 s−1 at 295 K and 250 K (figures 9(g)
and (h)). The performance of some of the pioneer-
ing studies on BP based FETs have been summar-
ized in table 2. These interesting reports pave the
way for further development of wafer-scale few-layers
phosphorene-based devices with broad applications
in versatile (opto)electronic devices and atomically
thin integrated circuits for the information industry.
Besides the quality and thickness of the semicon-
ductor thin film, the contact resistance also substan-
tially affects the performance of electronic devices. In
particular, the high contact resistance due to Schottky
barrier formation and contamination at the metal/BP
interface imposes severe limitations on the imple-
mentation of BP based devices for applications. The
contact resistance has a more pronounced effect on
short-channel devices because the contact resistance
is more influential than the channel resistance, lead-
ing the device performance to be limited by the
contact resistance. Also, the different contact metals
demonstrate very different behavior of BP based FET
devices, such as tuning the carrier type from n-type to
p-type or vice versa [175]. Du et al [176] presented an
intensive study on metal/BP interface from the device
perspective using high work function metals Ni and
Pd on BP based FETs. For the demonstration of the
contact resistance effect, several devices with channel
length scaling down from 3 µm to 100 nm have been
fabricated on the same BP flake (thickness 18.7 nm) as
demonstrated in figure 10(a). Although FET devices
fabricated using both Ni and Pd as source/drain elec-
trodes demonstrate Schottky behavior at BP/metal
interface. FET devices with Pd as source/drain elec-
trodes exhibited lower contact resistance than Ni con-
tacts. Figure 10(b) exhibits the dependence of con-
tact resistance with respect to back gate voltage for
both Ni and Pd contacts. It has also been observed
that the characteristics of FET devices could be altered
from intrinsic p-type to n-type behavior by proper
modulation of the channel length and bias. Perello
et al [177] demonstrated the transport behavior of
FETs fabricated on BP flakes ranging from 3 to 13 nm.
The effect of contact metal engineering on the BP
devices has been described using low work function
metal Al and high work function metal Pd. The thin-
ner BP flake (∼3.5 nm) shows unipolar n-type beha-
vior due to Schottky junction formation and large
contact resistance at Al/BP. However, the thicker BP
2D Mater. 9 (2022) 032001 V Chaudhary et al

Figure 9. (a) The transfer characteristics of a 5 nm thin phosphorene FET device with channel length and width equal to 1.6 and
4.8 µm, respectively. The inset shows optical image of a multi-terminal phosphorene device. Reproduced from [34], with
permission from Springer Nature. (b) Transfer characteristics of the few-layer phosphorene FET encapsulated with Al2 O3 layer.
(c) The mean normalized drain spectral density represents the effect of Al2 O3 passivation on noise reduction as a function of the
drain current. Reprinted with permission from [174]. Copyright (2014) American Chemical Society. (d) The variation in charge
carrier mobility in encapsulated and unencapsulated phosphorene FETs with respect to the ambient exposure time. Reprinted
with permission from [120]. Copyright (2014) American Chemical Society. (e) Variation of field-effect carrier mobility and
current ON/OFF ratio of the fabricated phosphorene FETs with temperature. (f) Variation of Hall mobility and carrier
concentration of 8 nm thin BP film with respect to temperature. Inset shows AFM image of Hall-bar device. Reproduced from
[151]. CC BY 4.0. (g) Variation of field-effect mobility and ON/OFF ratio resulting of different FET devices as a function of film
thickness. (h) Three-dimensional mapping of carrier mobility at 250 K obtained from device array having 25 FETs fabricated on
same 5 nm phosphorene layer. The bottom shows the optical image of the fabricated device array on 1 × 1 cm2 . Reproduced from
[152], with permission from Springer Nature.

Table 2. The summary of BP based FETs, including active layer thickness, performance parameters, and operating temperature.

Mobility Operating
Active layer/thickness (nm) (cm2 V−1 s−1 ) ON/OFF ratio temperature References

BP/10 984 105 RT [34]

BP/10 286 104 RT [33]
BP/5 205 105 RT [100]
BP/8 1200 105 RT [151]
1250 108 10 K
BP/5 213 103 295 K [152]
617 103 250 K
BP/3 BP/13 275 105 RT [177]
630 107 80 K
950 104 RT
BP/18.7 170 102 RT [174]
BP/8.5 400 103 RT [186]
BP/6.7 227 104 RT [179]
BP/15 310 104 RT [187]

13
2D Mater. 9 (2022) 032001 V Chaudhary et al

Figure 10. (a) Schematic view of device configuration with Ni and Pd contacts. (b) The variation of contact resistance for both Ni
and Pd contacts metals under various gate biases. Reprinted with permission from [176]. Copyright (2014) American Chemical
Society. (c) The variation of total device resistance with respect to channel length under different hydrogen concentrations.
(d) The variation of contact resistance with respect to hydrogen concentration. Reprinted with permission from [178]. Copyright
(2017) American Chemical Society.

flake (∼13 nm) demonstrates graphene-like ambi-
polar transport with mobility up to 950 cm2 V−1 s−1
at 300 K. On the other hand, high work function
metal Pd behaves as the same as in previous reports,
i.e. p-type behavior for thick flakes and symmetric
ambipolar transport for thin flakes with reduced con-
tact resistance. Further, Ma et al [178] reported the
ultralow contact resistance at the Pd/BP interface by
exposing the contacts to hydrogen mixed argon. In the
report, it has been argued that the hydrogen exposure
of Pd contacts forms Pd–H alloy, which significantly
increases Pd’s work function and reduces the Schottky
barrier height at the Pd–H/BP interface. Figures 10(c)
and (d) demonstrates the lowering of contact resist-
ance by increasing the hydrogen exposure concentra-
tion. This strategy has reduced the contact resistance
from ∼7.10 to ∼1.05 Ω mm for 5% hydrogen expos-
ure. Chang et al [179] described the lowering of con-
tact resistance down to 0.365 kΩ µm for germanium
doped metallic contacts. In the typical procedure,
Ge/Au contacts (10/60 nm) were evaporated on a
few layers BP followed by rapid thermal annealing to
250 ◦ C. The rapid annealing resulted in the forma-
tion of PGex alloy, which converted the Schottky con-
tact at the metal/BP interface to the Ohmic. Other
reports have also described the lowering of contact
resistance either by contact doping or thermal anneal-
ing [180–182]. These reports illustrate the import-
ance of selecting the right metal electrode and pro-
cessing analogy to understand the potential aspect of
BP in high-performance FETs.
Although, few-layer phosphorene demonstrates
commendable results in terms of carrier mobility
∼1000 cm2 V−1 s−1 at room temperature for micro
and macro-scale devices but still lower than that in
bulk BP, where the mobility approaches 15 000 and
50 000 cm2 V−1 s−1 , respectively, for electrons and
holes at low temperatures [33, 34, 60, 177]. How-
ever, the monolayer phosphorene demonstrated
very disappointing results. Cao et al [183] studied
the transport properties of BP ranging from 20 lay-
ers to monolayer and reported the room temper-
ature hole mobility ∼1200, 80, and 1 cm2 V−1 s−1 ,
respectively for tri layers, bilayers, and mono-
layer. Using numerical simulations, Rudenko et al
[184] reported an upper limit of carrier mobil-
ity in monolayer phosphorene. The simulation
was based on single- and two-phonon charge car-
rier scattering and resulted in the maximum elec-
tron/hole mobility ∼700/250 cm2 V−1 s−1 . Further,

14
2D Mater. 9 (2022) 032001
Gaddemane et al [185] studied the transport prop-
erties of monolayer phosphorene using Monte Carlo
and density functional theory (DFT) and reported
the mobility only up to 30 cm2 V−1 s−1 .
The issue of low mobility in very thin or mono-
layer phosphorene may be resolved using ultra-small
device geometry, i.e. reducing the channel length to
nanometric scale, which can enable ballistic quantum
transport. Miao et al [188] fabricated a few layers
BP based FETs with channel length 20 nm, and the
device exhibited an ON-state current of 174 µA µm−1
at V d 100 mV. Other studies with short channel
length BP nano devices demonstrated similar res-
ults, i.e. a fair on state current up to 300 µA µm−1
[176, 186]. Li et al [189] simulated the device per-
formance limit of the monolayer BP tunneling FETs
at 5 nm scale using ab initio quantum transport
calculations and predicted a high ON-state current
∼1113 µA µm−1 with a subthreshold swing around
101 mV dec−1 . The comprehensive theoretical invest-
igation of ballistic quantum transport in monolayer
BP based FETs devices demonstrates higher cur-
rent density and faster switching speed than con-
ventional 2D TMDs based devices [190, 191]. In a
recent report, a record-high drive current of ∼1.2
and 1.6 mA µm−1 has been achieved in BP tran-
sistors with 100 nm channel length at room tem-
perature and 20 K, respectively [192]. The highest
hole saturation velocity at room temperature was
found to be 1.5 × 107 cm s−1 . The ballistic trans-
port properties of this device have demonstrated a
record-high 36% and 79% ballistic efficiency at room
temperature and 20 K, respectively. Yin et al [193]
used atomistic quantum transport simulations and
the small-signal circuit model to optimize the fre-
quency limit of BP based FETs. The self-consistent
non-equilibrium Green’s function simulation estab-
lished that BP based FETs demonstrate saturation
behavior with an increase in drain voltage, in con-
trast to graphene FET, which results in >10 THz fre-
quencies for intrinsic f T and f max . Also, the contact
resistance, parasitic capacitance, and channel length
significantly affect both f T and f max . The simulation
results suggested that with precise engineering of FET
architecture parameters and contact resistance, BP
based FETs may approach near THz frequency range
(f T = 900 GHz; f max = 1.2 THz). However, the BP
based high-frequency FETs are still in infancy state
and, so far, experimentally demonstrate the frequency
response only up to f T = 17.5 GHz; f max = 14.5 GHz
for a short channel length of 250 nm [194]. Also,
few-layer phosphorene FETs demonstrated the giga-
hertz frequency operation with a cut-off frequency
of 12 GHz and a maximum oscillation frequency of
20 GHz [186].
Two-dimensional layered heterostructure-based
materials have played a crucial role in a vari-
ety of nanoelectronics devices because of their
multifunctional properties. Jeon et al [195] fabricated
15
V Chaudhary et al
junction-FETs with ZnO-wire/phosphorene het-
erojunction as the channel and demonstrated an
ON/OFF ratio as high as 104 . Following the great
promise of ZnO-wire/phosphorene heterojunction
in nanoelectronics, FET devices based on hetero-
structures of phosphorene and other semiconductors
would be of significant potential. In addition,
van der Waals heterojunctions of 2D atomic crys-
tals have drawn enormous interest because of
their excellent properties and potential electronic
applications. In the same order, Li et al [117]
designed phosphorene/h-BN/MoS2 heterojunction
and demonstrated the floating-gate-based FET device
with an appreciable program/erase ratio with tolerant
performance. Also, the complementary metal oxide
semiconductor (CMOS) inverter based on 2D BP
has been realized by constructing heterostructures
with other 2D materials like graphene and MoS2
[33, 196, 197]. Another breakthrough study came
with selective deposition of copper on phosphorene
flakes to generate the n-type channel, which enabled
the realization of a complementary inverter entirely
based on few-layer phosphorene [198].
In addition, few-layer phosphorene FETs demon-
strate intriguing features such as the velocity modu-
lation effect [199], Shubnikov–de Haas oscillations,
etc [200–204]. Also, few-layer phosphorene can be
used in flexible and wearable electronics due to
its unique mechanical properties, such as excellent
flexibility. The flexible ambipolar transistors of BP
with amplitude modulation and demodulation have
been reported by Zhu et al [187]. The encapsu-
lated BP-based ambipolar FETs on flexible polyim-
ide substrate exhibited maximum carrier mobility
∼310 cm2 V−1 s−1 with modulation exceeding three
orders of magnitude. The obtained carrier mobil-
ity is much higher than other TMDs and flexible
organic transistors.
5.2. Optoelectronic devices
The layer thickness-dependent direct electronic
bandgap makes phosphorene a promising material
for nanophotonic and optoelectronic applications as
well [100, 205–207]. Phosphorene fills the gap left by
other 2D materials such as graphene and TMDs as
well as the electronic band structure of phosphorene
can be changed through local mechanical geometry
modification for a more comprehensive spectral cov-
erage [208–211]. Due to its attractive properties,
BP and phosphorene have been utilized as a versed
material in many optoelectronic devices. The tunable
bandgap with optical anisotropy and substantial car-
rier mobility allows few-layer BP and or phosphorene
to be suitable for light sensing and optical imaging.
Buscema et al [43] demonstrated the photo-
detection behavior of phosphorene FETs from the
visible region of the spectrum to 940 nm with
a rise time of about 1 ms. They could achieve
a maximum photoresponsivity of 4.8 mA W−1
2D Mater. 9 (2022) 032001
Table 3. The summary of photodetectors realized on BP and its heterostructures including active layer thickness, performance
parameters, and operating wavelength.
Operating
Active layer (thickness) wavelength (nm)
BP (8 nm) 640
BP/MoS2 (22/0.65 nm) 633
BP/ReS2 (5/12 nm) 532
BP (5 nm) 405
BP (12 nm) 532
BP (7 nm) 830
MoS2 /BP/WSe2 532
(34/40/43 nm) 1550
BP (8 nm) 633
BP/MoS2 (10/4.8 nm) 532
BP/MoS2 (22/12 nm) 532
1550
for 640 nm illumination. Wu et al [206] repor-
ted few-layer phosphorene phototransistors having
extremely high photoresponsivity (∼9 × 104 A W−1 )
at a source-drain voltage of 3 V in the ultravi-
olet spectral region. Another few-layer phosphorene-
based phototransistor operating in the mid-infrared
range with a responsivity of 82 A W−1 was repor-
ted by Guo et al [211]. The noise measurements
showed that this phototransistor could sense mid-
infrared radiation even in the pico-watt range. Fur-
ther, single-pixel phosphorene photodetectors have
also been fabricated for near-infrared imaging [212].
Engel et al [213] developed multispectral high-
resolution imaging devices using few-layer phos-
phorene. This device was able to produce diffraction-
limited optical images with submicron resolution.
An exciting application of few-layer phosphorene has
been observed in waveguide-integrated gate-tunable
photodetectors with a telecom band’s response band-
width of more than 3 GHz [214]. Due to the aniso-
tropic properties of few-layer phosphorene, it has
been successfully exploited in polarization-sensitive
photodetection as vertical p–n junction assembly and
heterostructure with other conventional 2D semicon-
ductors [215–218]. The performance of photodetect-
ors based on BP and its heterostructures with other
2D materials has been presented in table 3.
Phosphorene can be employed as an efficient
material in solar cells due to its broadband light-
absorbing properties. In particular, it has been used
with other semiconductor materials in van der Waals
heterostructure configuration to fabricate hetero-
junction excitonic solar cells [216–221]. However,
interfacial band alignment is difficult to achieve
when phosphorene is used in solar cells, although
few interesting reports are available on the hetero-
structures of phosphorene with MoS2 and GaAs for
solar cells [220, 221]. Theoretically, the monolayer
phosphorene/TiO2 heterostructure showed excellent
photovoltaic properties leading to good power con-
version efficiency at the device scale [222, 223]. In
some reports, few-layer phosphorene has also been
16
V Chaudhary et al
Specific detectivity
Responsivity (A W−1 ) (Jones) References
4.8 × 10−3 103 [43]
0.418 — [196]
8 — [49]
9 × 104 1013 [206]
82 — [211]
0.018 — [212]
6.32 1.25 × 1011 [226]
1.12 2.21 × 1010
4.3 × 106 — [227]
0.17 — [228]
22.3 3.1 × 1011 [229]
153.4 2.13 × 109
employed in multilayer excitonic solar cells. The
application of liquid exfoliated phosphorene sheets
in single-walled carbon nanotube/Si heterojunction
excitonic solar cells has drastically improved the
power conversion efficiency (9.37%) by enhancing
the rate of exciton formation and charge carrier sep-
aration [224]. Recently, Wang et al [225] reported the
role of BP on the photostability of methyl ammonium
lead iodide (MAPbI3 ) perovskite solar cells. The
MAPbI3 /BP solar cells retained 94% of their initial
performance up to 1000 h of continuous illumina-
tion under the N2 atmosphere. Also, BP inhibited the
defect formation caused by Pb and slowed down the
charge recombination rate. These few reports of phos-
phorene/BP related to photovoltaics suggest its signi-
ficance for further improvement to get even higher
performance with a broadband response.
5.3. Sensors
Due to the large surface to bulk ratio, the 2D mater-
ials have been intensively investigated for gas sens-
ing applications. Compared to other competitors like
graphene and MoS2 , phosphorene is enriched by its
high carrier mobility, direct bandgap, and lone elec-
tron pair, which pave the way for efficient sensing
properties. In theoretical reports, it has been estab-
lished that phosphorene has a very high tendency to
bind with NO and NO2 molecules, making it suitable
for sensing these highly toxic gases [230]. In general,
the gases cause molecular doping on the phosphorene
surface mediated by the charge transfer interaction
between the guest molecule and phosphorene surface,
which leads to a measurable resistance change in the
phosphorene film.
Abbas et al [231] reported the chemical sens-
ing of NO2 using a multilayer BP FET device as
a sensor. The fabricated sensing device exhibited
increased conduction upon NO2 exposure and clas-
sic sensitivity for NO2 detection down to 5 ppb.
Cui et al [170] developed a FET sensor device
using phosphorene nanosheets of thickness 4.8 nm
(figure 11(a)). The sensor demonstrated an ultrahigh
2D Mater. 9 (2022) 032001 V Chaudhary et al

Figure 11. (a) AFM images of phosphorene nanosheet sensor device. (b) The response curves of relative conductance change
versus time for NO2 sensing from 20 to 1000 ppb under drain-source voltage of 0.6 V. The dashed blue line represents the
‘ON/OFF’ cycle of NO2 gas. Reproduced from [170]. CC BY 4.0. (c) The sensing response of humidity sensor under multiple
exposures of water vapor. The blue curve represents the sensing response from the prepared device, and the red curve represents
the sensing response of the same device after 3 months of exposure to ambient conditions. (d) The drift behavior of the sensor
under prolonged exposure to 35% and 83% relative humidity (RH) at 25 ◦ C. Reprinted with permission from [233]. Copyright
(2015) American Chemical Society. (e) The sensing performance of pristine and Pt-functionalized BP for different gases
(1000 ppm toluene, hexane, ethanol, acetaldehyde, 1% H2 , and 100 ppm of NO2 ). (f) The response of Pt-functionalized BP and
pristine BP for various concentrations H2 gas. Reprinted with permission from [171]. Copyright (2017) American Chemical
Society.

Table 4. Gas sensing performance (NO2 gas) of BP based chemical sensors.

Operating
Active layer temperature (nm) Sensitivity (%) Response time (s) Recovery time (s) References

BP/NO2 RT — 280–350 840 [231]

BP/NO2 RT 190 — — [171]
BP/NO2 RT 95 200 — [232]
BP/NO2 RT 60 — 200 [238]
BP–In2 O3 /NO2 25 — 130 290 [239]
CuO–BP/NO2 RT 20 4 56 [240]
ZnO–BP/NO2 — — 2 16 [241]

sensitivity of ∼190% at 20 ppb for NO2 under
ambient conditions at room temperature, as demon-
strated in figure 11(b). In a comparative study of sens-
ing properties of 2D materials, BP exhibited superior
sensing behavior for NO2 over graphene and MoS2
[232]. The sensing parameters of BP based gas sensors
for NO2 gas have been listed in table 4.
Mayorga-Martinez et al [234] studied the vapor
sensing properties of layered BP and presented an
excellent methanol sensor by using electrochemical

17
2D Mater. 9 (2022) 032001
impedance spectroscopy as the detection tool. The
device showed the capability of selective detection
of methanol vapor down to 28 ppm. Further, Yasaei
et al [233] demonstrated an excellent humidity sensor
based on BP with stability for as long as 3 months.
Figures 11(c) and (d) presents the humidity sensing
response of the fresh and 3 months old devices. It has
been found that the sensing response of a 3 months
old device is almost the same as that of a freshly
prepared device. Also, a selective and ultrasensitive
response for humid air was observed with a trace-level
detection capability. The BP has also been explored
for hydrogen sensing, as illustrated in figures 11(e)
and (f). The efficient hydrogen sensing devices based
on BP have been obtained via functionalization of BP.
with noble metals like Au and Pt [169, 170]. Besides
chemical sensing, phosphorene has also shown out-
class results in ion sensing and biosensing [235–237].
These studies open the way for using BP or phos-
phorene films in many potential chemical/biosensing
applications.
5.4. Biomedical applications
Two-dimensional nanomaterials have shown prom-
ising performance in optical imaging, targeted drug
delivery, phototherapy, biosensing, and other bio-
medical fields because of their unique properties
[242–249]. The layer-dependent tunable bandgap of
phosphorene makes it able to interact with a large
region of the electromagnetic spectrum, which may
benefit cancerous cell apoptosis. Furthermore, the
puckered layer structure of phosphorene provides
a suitable surface area that may interact with bio-
active molecules, several drugs, metal atoms, and
fluorescent molecules. The non-covalent functional-
ization of phosphorene with these bioactive materi-
als or drugs renders several advantages in the med-
ical field, such as biomolecule detection, targeted
drug delivery, cell imaging, and cancer therapy [242].
Moreover, compared to other conventional 2D nan-
omaterials, phosphorene shows smaller cytotoxicity
and enhanced biodegradability in the human body.
These versatile properties of phosphorene attracted
the interest of scientists for its applicability in mul-
tifunctional biomedical applications.
Sun et al [248] examined few-layer phosphorene
for the antibacterial properties and found excel-
lent antimicrobial response for Escherichia coli (E.
coli) and Staphylococcus aureus (S. aureus). Com-
pared to graphene and MoS2 , few-layer phosphorene
has shown noticeable antibacterial strength against
both E. coli and S. aureus with a killing ratio as high
as 99.2%. Liu et al [250] functionalized the phos-
phorene nanosheets with Pt-based anticancer drugs
and demonstrated the application in chemo-cancer
therapy via self-stabilization of the drug. The phos-
phorene nanosheets encapsulated with polyethyl-
ene glycol exhibited multifunctional drug-delivery
with classic biocompatibility and manifested good
18
V Chaudhary et al
results in acute lymphoblastic leukemia therapy
[251]. Apart from the drug-delivery and antibacterial
activity, phosphorene and its functionalized
derivatives revealed promising impressions in
biosensors [252–255].
6. Summary and future scope
The present review comprehensively explored the
progress of phosphorene’s synthesis, properties, and
application in various fields. In summary, it is clear
that phosphorene and its derivatives play a signi-
ficant role in the development of advanced mater-
ials due to their excellent optical, electronic, and
mechanical properties that exhibit great potential in
many applications, including high-speed electronic,
optoelectronic, sensor devices, and biomedical fields.
However, the research on the properties and applica-
tions of phosphorene is still at a very early stage; many
important unresolved issues remain to be addressed
before successful practical applications of this mater-
ial. There is still a need to develop the control on the
layer number and the lateral size regarding the syn-
thesis. As an example, mechanical and liquid exfo-
liation are attractive methods of synthesizing phos-
phorene. Still, the phosphorene sheet produced by
these techniques has drawbacks such as partial glue
retention, small flake size, and structural defects that
affect the overall device performance.
The wet-chemical and CVD techniques have
played an essential role in manufacturing other
2D materials with high quality, but these methods
have not yet been effectively used in phosphorene
synthesis. However, synthesizing high-quality phos-
phorene by bottom-up routes will open a big room
with several benefits for exploring the fundamental
properties, applicability, and further device-scale
modifications. Current research on phosphorene
needs a technological breakthrough in bottom-up
synthesis, which may produce wafer-scale high-
quality monolayer phosphorene sheets. It may start
new directions that have to be investigated for novel
physical phenomena and device development. Even
though research on phosphorene has just started, it
is worth mentioning that phosphorene has already
been employed in several device applications such as
transistors, memory devices, optoelectronic devices,
and sensors. After its discovery, phosphorene and its
derivatives have been successively harnessed in FETs
thanks to their extensive range of desired features,
such as tunable bandgap and high mobility. The FETs
based on few-layer BP have been realized on rigid
and flexible substrates with excellent performance,
i.e. mobility up to 1000 cm2 V−1 s−1 and ON/OFF
ratio of 103 –105 . Therefore, it can be expected that
few-layer BP or phosphorene-based FETs may per-
form even better by device architecture modifica-
tions, interface engineering, etc.
2D Mater. 9 (2022) 032001
Recently, vertically stacked layer by layer van
der Waals heterostructures of multiple 2D materials
have inaugurated a new avenue in materials science
to develop novel architectures for numerous func-
tionalities. The functionalization/heterostructures of
phosphorene with other members of the 2D fam-
ily may provide unprecedented success in many
fields, especially the development of new types
of electronic and optoelectronic devices. Moreover,
defect engineering, such as the intentional creation
of vacancies, antisites, and dislocations, may tailor
the fundamental properties of the phosphorene as
per requirement.
With fascinating properties such as controllable
bandgap, ambipolar charge transport, high mobil-
ity, and flexibility, phosphorene and its derivat-
ives may undoubtedly play a crucial role in various
components of optoelectronics, including solar cells,
photodetectors, and light emiting diodes (LEDs).
Phosphorene has found its unique place among
chemical/biological sensors also. Apart from sensing,
early experiments have also shown its application in
targeted drug delivery and chemotherapy. However,
there is still a big room for improvement via function-
alization, which may make phosphorene more suit-
able to exploit in these applications. Finally, the envir-
onmental stability of phosphorene imposes severe
limitations on its applicability in modern technolo-
gies. The issue of degradation of phosphorene needs
serious attention and must be solved before its utiliz-
ation in existing and possible future applications.
Data availability statement
No new data were created or analyzed in this study.
Acknowledgments
This work has been supported by OCP project
Grant AS70 ‘Towards phosphorene-based materials
and devices’ P N and A E F would like to fur-
ther acknowledge support from ERC Grant under
the European Union’s Horizon 2020 Research and
Innovation Programme (GA No. 714850), as well
as the Grant LTAUSA19060 INTER-EXCELLENCE
Programme, funded by the Ministry of Educa-
tion, Youth and Sports of the Czech Republic.
A E F would like to further acknowledge the sup-
port of the Chair ‘Multiphysics and HPC’ led by
Mohammed VI Polytechnic University, sponsored
by OCP.
Conflict of interest
The authors declare no conflict of interest.
19
V Chaudhary et al
ORCID iDs
Vivek Chaudhary  https://orcid.org/0000-0003-
1461-4073
P Neugebauer  https://orcid.org/0000-0001-7095-
6401
S Lahbabi  https://orcid.org/0000-0003-1991-4534
A El Fatimy  https://orcid.org/0000-0001-6500-
7762
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