Projection Micro Stereolithography Based 3 DPrintingand Its Application

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Projection Micro Stereolithography Based 3D Printing and Its Applications
Article in International Journal of Extreme Manufacturing · April 2020

DOI: 10.1088/2631-7990/ab8d9a
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Projection Micro Stereolithography Based 3D Printing and Its

Applications
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International Journal of Extreme Manufacturing
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Projection Micro Stereolithography Based 3D Printing and
Its Applications
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Journal: International Journal of Extreme Manufacturing
Manuscript ID IJEM-110057.R1
Manuscript Type: Topical Review
Date Submitted by the

06-Apr-2020
Author:
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Complete List of Authors: Ge, Qi; Southern University of Science and Technology, Department of
Mechanical and Energy Engineering
Li, Zhiqin; BMF Material Technology Inc.
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Wang, Zhaolong; Hunan University, State-Key Laboratory of Advanced
Design and Manufacturing for Vehicle Body
Kowsari, kavin; Massachusetts Institute of Technology, Department of
an
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Mechanical Engineering
Zhang, Wang; Singapore University of Technology and Design, Pillar of
Engineering Product Development
He, Xiangnan; Southern University of Science and Technology,
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Department of Mechanical and Energy Engineering

Zhou, Jianlin; BMF Material Technology Inc.
Fang, Nicholas ; Massachusetts Institute of Technology, Department of
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Mechanical Engineering
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Projection Microstereolithography, Multiscale 3D Printing, Multimaterial

Keywords:
3D Printing
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https://mc04.manuscriptcentral.com/ijem-caep
Page 1 of 34 International Journal of Extreme Manufacturing
1 Projection Micro Stereolithography Based 3D Printing and Its Applications

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6 Qi Ge 1,*, Zhiqin Li 2, Zhaolong Wang 3,*, Kavin Kowsari 4, Wang Zhang 5, Xiangnan He 1, Jianlin Zhou 2,
7 Nicholas X. Fang 4,*
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1. Department of Mechanical and Energy Engineering, Southern University of Science and Technology,
11 Shenzhen, Guangdong, China, 518055
12 2. BMF Material Technology Inc., Shenzhen, 518110
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3. State-Key Laboratory of Advanced Design and Manufacturing for Vehicle Body, College of Mechanical
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15 and Vehicle Engineering, Hunan University, Changsha, Hunan, China, 410082
16 4. Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, MA, United
17 States, 02139-4307
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19 5. Digital Manufacturing and Design Centre, Singapore University of Technology and Design, Singapore,
20 487372
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Corresponding authors: Q.G.: geq@sustech.edu.cn; Z.W.: zhaolongwang@hnu.edu.cn; N.X.F.:
24 nicfang@mit.edu.
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International Journal of Extreme Manufacturing Page 2 of 34
1 Abstract: Projection Micro Stereolithography (PμSL) is a high-resolution (up to 0.6 μm) 3D printing
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3 technology based on area projection triggered photopolymerization, and capable of fabricating complex 3D
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5 architectures covering multiple scales and with multiple materials. This paper reviews the recent
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7 development of the PμSL based 3D printing technologies, together with the related applications. It
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introduces the working principle, the commercialized products, and the recent multiscale, multimaterial
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printing capability of PμSL as well as some functional photopolymers that are suitable to PμSL. This review
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paper also summarizes a few typical applications of PμSL including mechanical metamaterials, optical
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components, 4D printing, bioinspired materials and biomedical applications, and offers perspectives on the
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16 directions of the further development of PμSL based 3D printing technology.
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1 1. Introduction
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3 In contrast to the subtractive nature of conventional machining, additive manufacturing (also known as 3D
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5 printing), physically reproduces parallel slices of arbitrary design files by first decomposing the object’s
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7 shape into a series of parallel slices. 3D printing methods fabricate highly complex 3D objects from
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9 computer-aided design (CAD) models by sequentially adding material in the layer-by-layer fashion [1, 2],
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11 which minimizes the material waste, and is applicable to a variety of different materials such as polymers,
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13 metals, ceramics, composites, and others. Since its invention, various modalities of 3D printing methods
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15 have been evolved. New methods are continually presented to overcome challenges encountered in existing
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17 methods. So far, in terms of application and market share, 3D printing has spread into various manufacturing
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19 areas including electronics, medical, automotive, and aerospace [2]. A report from the United Parcel Service
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21 (UPS) and the Consumer Technology Association (CTA) projects forecasts that the 3D printing industry will
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exceed $21 billion by early 2020s [3], which supports the notion that continued progress in this sphere is
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crucial to global economic competitiveness.
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Consequently, many 3D printing techniques are now available, which differ in the manner layers that
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29 are deposited, operating principles, and the materials scope. The following broad categories constitute the
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31 main methods available, some of which are as follows and described below: fused deposition modeling
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33 (FDM), direct ink writing (DIW), inkjet, stereolithography (SLA), selective laser sintering/melting
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35 (SLS/SLM), two-photon polymerization (TPP) as well as digital light processing (DLP).
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Among all 3D printing technologies, fused deposition modelling (FDM) is the most common
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technology due to its low cost and simplicity [4-6]. In FDM, the heated printing nozzle melts or softens
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41 thermoplastic filament and extrude it on a build tray in a layer-by-layer manner to fabricate 3D structures.
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The extruded filament solidifies due to phase transition (mainly crystallization) after it leaves the heated
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45 nozzle.
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48 Similar to FDM, direction ink writing (DIW) is another extrusion-based 3D Printing technology [7-12].
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50 Different FDM that uses thermoplastics, a DIW printer deposits viscoelastic inks which are shear thinning
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52 materials whose viscosity varies from ~ 1 kPa∙s to ~ 1Pa∙s after increasing the pressure from 1/s to 100/s
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54 [13]. In order to maintain the desired printed shapes on the build tray, sufficient shear elastic modulus is
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56 needed for the thinning materials exiting from the nozzle. For this purpose, thinning agents such as clay
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58 need to be added to modify the respective rheological property of inks.
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60 Selective laser melting (SLM) and selective laser sintering (SLS) are two powder- bed-fusion based 3D
printing technologies [14-17]. In a SLM/SLS printer, there are fine powders tightly packed in the printing
1 bed. During printing, a laser beam selectively fuses the powders to 2D pattern. The subsequent layer is
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3 processed by rolling a layer of powders on top of previous layers and fusing them together. However, it
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5 should be noted that SLS is mainly used to process polymers, metals and alloy powders, while SLM is only
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7 suitable for certain metals such as steel and aluminum.
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9 Inkjet is a 3D printing method that fabricates 3D structures by using a thermal or piezoelectric
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11 technology to deposits nano/microscale low-viscosity ink droplets on a build tray by using [5, 16]. An inkjet
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13 printer combines an ink-jetting head and an ultraviolet (UV) light source in one platform. During printing,
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15 the ink-jetting head selectively deposits ink droplets on the build tray to form 2D patterns which are
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17 immediately solidified upon the illumination of the UV light source.
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20 Different from the above-mentioned 3D printing technologies, the high-resolution 3D printing
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techniques are realized through localized photopolymerization that precisely transfers liquid polymer resin
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to solidified voxels. Those high-resolution 3D printing technologies mainly includes two-photon
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polymerization (TPP) [18-22], stereolithography (SLA) [16, 23-27], digital light processing (DLP) based 3D
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printing [16, 28-39]. TPP uses an ultrafast pulsed laser to generate a very high flux of photons in a small
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29 temporal and spatial volume. Since these photons are at longer wavelengths (780-820 nm), the polymer resin
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31 can be solidified only by absorbing two photons at the same time, which allows TPP to achieves sub-micron
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33 features [40]. As the first 3D printing technology, SLA was invented in 1986 [41]. In SLA, a rastering laser
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35 is used to selectively polymerize a liquid polymer resin in a layer-by-layer manner to fabricate 3D objects.
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37 TPP and SLA are both laser-scanning based 3D printing technologies, therefore relatively slow as they
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39 locally photopolymerize polymer resin based on point-light-source illumination.
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42 Different from TPP and SLA, DLP based 3D printing performs the localized photo-curing through
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44 projecting 2D UV patterns on the surface of liquid polymer resin. DLP that combines the feature of
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46 high-resolution with fast-speed. The recent advances in DLP based 3D printing generate various advanced
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techniques including projection micro stereolithography (PµSL) for high-resolution 3D printing [28-31],
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continuous liquid interface production (CLIP) for fast-speed 3D printing (1000 mm/h in z-direction) [38], as
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well as high-area rapid printing (HARP) for fast-speed (431 mm/h in z-direction), large volume 3D printing
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(38 cm × 61 cm × 76 cm in 1hour and 45 min) [39].
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56 Besides the above-mentioned 3D printing technologies which have been widely accepted by the
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58 research and industry communities, there are a few emerging technologies that pushes the boundary of 3D
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60 printing speed. Electrohydrodynamic (EHD) 3D printing achieves three to four orders of magnitude faster
than the other techniques providing equivalent feature sizes [42, 43]. Tomographic volumetric additive
1 manufacturing fabricates a centimeter scale object within tens of seconds, which also indicates consistent
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3 advantages of fast speed and high resolution [44, 45]. These technologies will bring 3D printing to a new
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5 stage once they are more mature.
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7 In general, there is the contradictory relation between printing area and printing resolution. It means
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9 that to print structure with higher resolution needs to reduce the printing area into a smaller one. As shown in
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11 Figure 1, the above introduced 3D printing technologies offer different printing resolutions, and therefore
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13 cover the corresponding printing areas. For example, TPP offers ~100 nm ultrahigh printing resolution
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15 [18-22], but it only covers relatively small printing area ranging from 10 μm × 10 μm to 2.2 mm × 2.2
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17 mm despite of the recent development of the multiscale printing approach that combines TPP with digital
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19 micromirror device (DMD) [22]. In contrast, DIW is a versatile 3D printing technology which can not only
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be applied to the bio-related 3D printing that covers printing area of 30 mm × 30 mm with printing
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resolution of 200 μm [8], but also be used to print constructions in the printing area up to 10 m × 10 m with
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the printing resolution of 50 mm [10, 11]. Compared with other 3D printing technologies, DLP based 3D
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printing technologies cover a broader spectrum of printing resolutions from 0.6 μm to 90 μm by adjusting
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the magnification of the projection lens. Within the DLP based 3D printing technologies, there is a specific
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30 technique termed “Projection Micro Stereolithography (PμSL)” which is capable of printing complex 3D
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32 structures with higher resolution ranging from 0.6 μm to 30 μm and relatively wide printing area up to ~90
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34 mm × 50 mm [28-31, 36, 46, 47]. The detailed summary of the printing resolution-area relation of different
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36 3D printing technologies is presented in Table 1.
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57 TPP DLP SLA DIW INKJET FDM SLS&SLM

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59 Figure 1. The diagram summarizes the printing resolution and printing area relation of TPP [18-22], DLP
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[16, 28-39], SLA [16, 23-27], DIW [7-12], inkjet [5, 16], FDM [4-6] as well as SLS&SLM [14-17].
Table 1. Summary of the printing resolution-area relation of different 3D printing technologies.

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2 Technology Resolution (μm) Printing Area (mm2) Reference
3 0.08 0.0064 [22]
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5 0.1 0.000144 [19]
6 TPP 0.12 0.0001 [20]
7 0.13 4.84 [18]
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9 0.16 12.25 [21]
10 0.6 2 [28] (PμSL)
11 1.3 15 [29] (PμSL)
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13 2, 10 8.2944, 2500, 4888 [32] (PμSL)
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14 5 25 [30] (PμSL)
15 5 2500 [31] (PμSL)
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DLP 30 768 [36] (PμSL)
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18 7.6 234.135 [33]
19 13.68 147.2451 [34]
20 35, 90 5040, 32969.5 [37]
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23 65 8760.96 [16]
24 75, 125 62500, 144400, 487500, 1125000 [16]
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26 85, 140 21025 [27]
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SLA
120, 200, 800
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30 150 5476 [8]
31 200 900 [9]
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34 9000 1800000 [10]
35 50000 100000000 [12]
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34, 68 52540, 191100, 55130 [16]
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38 42, 85 116964, 191100, 800000 [5]
39 127, 254, 330,
40 64516, 144130, 90170, 144130,557540 [5]
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42 300 49200 [4]
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1000 1010025 [6]

44 55, 100 9604, 40000, 84100 [15]
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46 100 10000, 250000 [16]
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47 100 160000 [17]
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140, 150, 500 15625, 78400, 140000, 84100 [14]
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53 This review paper aims to summarize the recently advanced PμSL based 3D printing technologies. In
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55 Section 2, we introduce the technological advancements of PμSL based 3D printing including the working
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57 principle, commercialized products, and recent developments in multiscale, multimaterial and

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59 multifunctional 3D printing. Section 3 summarizes the developments in functional photopolymers that are
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used in PμSL and other DLP based 3D printing technologies. In Section 4, we introduce the typical
applications of PμSL based 3D printing including mechanical metamaterials, optical components, 4D
1 printing, bioinspired materials as well as biomedical applications. Finally, Section 5 concludes the article
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3 and provides perspectives on the directions of the further development of PμSL based 3D printing
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5 technology.
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8 2. PµSL based 3D Printing Technologies
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10 The early version of high-resolution PμSL apparatus was developed by Sun and his coworkers in 2005 by
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12 using the digital micromirror device (DMD) as the dynamic mask [28]. As shown in Figure 2a, the PμSL
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14 based 3D printer fabricates a complex 3D microstructure in a layer-by-layer manner. During printing
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16 process, a computer aid design (CAD) model is first sliced into a sequence of 2D digital patterns. Then,
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18 these 2D patterns are transferred to the DMD chip which modulates the UV light illuminated on it. The
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20 shaped UV lights with the corresponding defined 2D patterns pass through a reduction lens that projects the
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22 2D images on the resin surface with a reduced feature size. The patterned UV irradiation triggers the
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24 localized photopolymerization on the resin surface, which forms a layer of the printed structure. The
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26 translational stages lowers the printing platform, and the UV projection continues to print the subsequent
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layer. This process proceeds iteratively until the entire structure is fabricated. In order to reveal the
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30 underlying mechanisms for PμSL, the authors developed a numerical model based on diffractive optics. The
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32 model justified the role of UV doping due to its ability of effectively reducing the curing depth without
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34 sacrificing the chemical property of the resin. The first developed PμSL system was able to fabricate highly
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complex 3D microstructures, such as a micro-spring array (Figure 2b), and a thread with the feature size as
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small as 0.6 μm (Figure 2c).
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40 To further improve the performance of the PμSL system, Zheng et al. optimized the system design by
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42 using liquid crystal on silicon (LCoS) chip as the dynamic mask, and a UV LED as the light source
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44 (Figure 2d) [29]. The authors improved the light projection uniformity by taking advantage of the grayscale
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46 capability of the LCoS spatial light modulator. They carried out the experimental parametric study to
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48 investigated the effects of various process control variables, and concluded that the photo absorber
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50 concentration and optical intensity are the two most important processing parameters. In addition, the
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52 ambient oxygen concentration was precisely controlled by enclosing the UV curable resin bath in an
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54 environmental chamber to eliminate the effect of oxygen inhabitation (Figure 2d). The modified PμSL
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56 system is capable of fabricating arbitrary 3D overhanging structures with highly complex geometries such as
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58 octet truss unit cell (Figure 2e) and porous materials (Figure 2f).
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1 a UV beam d Light slit Pellicle beam splitter

2 Beam Elevator
Beam
LCOS splitting
3 delivery cube
4 Digital micro-
5 mirror display Projection
z Difusser CCD Reduction
optics
6 lens
LED
7 CAD Translation
y O2 sensor
8 Projection for stage
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9 Reflection for
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x UV curable solution
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UV curable resin
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Figure 2. PµSL based 3D Printing Technologies. (a)-(c) The first proposed PµSL based 3D printing. [28] (a)
24 Schematic of the system design. (b) micro coil array with the coil diameter of 100 µm and the wire diameter
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25 of 25 µm. Scale bar: 200 µm. (c) An ultra fine thread with the diameter of 0.6 µm. (d)-(f) The PµSL system
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using LCoS chip as the dynamic mask. [29] (d) Schematic of the system design. (e) Octet-truss unit cell.
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Scale bar: 490 µm. (f) Porous structure with tetrakaidehedron unit cell architecture. Scale bar: 640 µm.
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31 In 2018, a micro/nano fabrication company-BMF Materials Technology Co, Ltd. commercialized the
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33 PμSL based 3D printing technologies [32]. It offers two high-resolution large-area printing options: (i) 2 μm
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per pixel with 50 mm×50 mm printing area (nanoArch S130) and (ii) 10 μm per pixel with 94 mm×52 mm
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printing area (nanoArch S140). The system design is presented in Figure 3a. In order to accurately control
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the layer thickness, a pre-stretched transparent and anti-sticky perfluoroalkoxy (PFA) membrane is placed
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between the surface of resin and projection lens. Before printing, a high-resolution stage coordinated with a
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42 CCD camera automatically moves the membrane to a position where the focal plane of the projection lens
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44 coincides with the wet surface of the membrane. The multiple-projection stitching process is adopted to
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46 realize large-area printing. The total fabrication area can be further divided into multiple subareas which are
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48 smaller than a single projection. When a layer of subarea is printed, the X and Y stages move horizontally
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50 for the fabrication of a neighboring subarea. Since its debut, the nanoArch series have been successfully
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52 used in various engineering applications including mechanical metameterials (Figure 3b-c), biomedical
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54 devices (Figure 3d-f), micro mechanical devices (Figure 3g-h), precision structural parts, and others [32, 48,
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56 49].
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Mechanical metamaterials
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2
a CCD b c
3 DMD
4 Beam-
splitter
5 UV LED 88 mm 20 mm 2 mm ~165 μm
6 Projection Biomedical devices Precision structural
lens
7 d e f i parts
8 Film Printing
model
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9 Film
10 fixture
11 Scraper Platform
12 Resin stage Micro mechanical devices
13 Film g Upper compression head
Horizontal Top h
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14 beams shuttle
j
X stage Printing
15 platform
Inclined
beams
16 Y stage Sample stage shuttles
500 μm
17 Lower compression head
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19 Figure 3. Commercialized high-resolution large-area PμSL based 3D printing system and its engineering
20 applications. [32] (a) Schematics of a PμSL 3D printing system. (b) and (c) Application in mechanical
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21 metamaterials. (b) The printed mechanical metamaterial in the octet truss form. Scale bar: 100 μm. (c) The
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mechanical metamaterial in the hierarchical structure form. Scale bars from left to right: 2 mm, 200 μm, and
24 500 μm respectively. (d)-(f) Application in biomedical devices. (d) Tilted Microneedles for drug injection.
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25 Scale bar: 1 mm. (e) Micro buckyball for cell cultivation. Scale bar: 50 μm. (f) Drainage Nail for Glaucoma.
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Scale bar: 500 μm. (g) and (h) Micro Mechanical Devices (MMDs). (g) A MMD for in-situ tensile testing of
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micro/nanowires [50]. (h) Micro spring array with 20 μm diameter for each spring. Scale bar: 100 μm. (i)
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29 and (j) Precision structural parts. (i) Micro fiber connector with minimum groove edge thickness of 80 μm.
30 Scale bar: 5 mm. (j) Micro socket with approximately 1700 trapezoidal hole arrays. Scale bar: 12.5 mm.
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33 To further extend the fabrication capability of the PμSL based 3D printing, several efforts have been
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35 made to realize multiscale, multimaterial and multifunctional 3D printing in the past few years. As shown in
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37 Figure 4a, Zheng et al. developed a large area projection microstereolithography (LAPµSL) that combines a
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39 traditional DMD based PµSL system with a coordinated optical scanning system [31]. The system combines
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41 a galvanometric mirror with a customized scanning lens to project the light pattern from the DMD onto the
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43 UV curable polymer resin surface, and therefore is capable of fabricating microstructures with feature size
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45 span over four orders of magnitude within only a few hours. Combining LAPµSL with electroless nickel
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47 deposition, the authors successfully fabricated the multiscale metallic metamaterials with various 3D
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49 features from nanometers to centimeters (Figure 4b). Inspired by the computer numerically controlled (CNC)
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51 accumulation process, Yang et al. developed another PµSL based multiscale 3D printing approach -
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53 immersed surface accumulation based 3D (ISA-3D) printing where the light guide tool consisting of optical
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55 fibers and objective lens is the key component (Figure 4c) [51]. The light guide tool is merged inside a tank
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of UV curable resin for continuous 2D light beam projection. Combining with the 5-axis movement of the
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59 light guide tool and the dynamically controlled light beam projection, the ISA-3D printing system enables
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the fabrication of microscale features on the surface of a macroscale object. It is capable of projecting UV
patterns on a 3.67 mm × 2.75 mm with resolution of 2.5 μm per pixel. Using the ISA-3D system, the authors
1 successfully printed bioinspired super-hydrophobic structure with 2.5 μm feature size on centimeter scale
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3 curved surface.
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7 a c Lens
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9 Scanning
Lens
optics
10 Camera
11 Spatial light Lens
12 modulator (SLM) Customized
Rotating optical fiber
13 UV LED at
focusing lens
Optical microscope
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14 405 nm
15 Projecting image Light guide tool z
16 Z axis
pattern from SLM Optical fiber β x
17 elevator High resolution and y α
Tank
18 large 3D printed object
19 Eglass/MWCNT
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24 200 μm
Eggbeater Optical
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29 Hierarchical Hierarchical lattice Hierarchical 200 μm
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32 Figure 4. PµSL based multiscale 3D printing. (a)-(b) Large area projection microstereolithography
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34 (LAPµSL) multiscale 3D printing. [31] (a) Schematic of the LAPµSL printing system that combines a
35 traditional DMD based PµSL system with a coordinated optical scanning system. (b) Snapshots of a
36 hierarchical mechanical metamaterial. Scale bar is 80 µm. (c) Schematic illustrations of the ISA-3D printing
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system. Inserts show the magnification of light guide tool, optical fiber with projected 2D micro patterns,
39 models and SEM image of the 3D-printed eggbeater arrays. [51]
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42 Multimaterial 3D printing is a desired capability which allows users to fabricate heterogenous 3D
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44 structures that have the inaccessible functionalities by single material printing such as 4D printing [36, 52,
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46 53], negative thermal expansion [54], organ-like structures [55], and others [56-58]. Among all the 3D
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printing technologies, the multimaterial fabrication can be easily realized in FDM and DIW through simply
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adding extra printing nozzles to deposit different materials, and inkjet 3D printing technology in which
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photocurable resin is jetted over a surface through micro-nozzles followed by curing with UV light.
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However, compared with the above discussed 3D printing technologies, the development of multimaterial
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55 PµSL based 3D printing systems remain comparatively limited due to the difficulties of exchanging polymer
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57 resins [46, 47]. To address this, Kowsari et al. built a high-resolution, high-speed, and high-efficiency PµSL
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59 based multimaterial 3D printing system that used a translationally moved glass plate to deliver different
60
material puddles to realize the fast-speed material exchange, and employed an air jetting based cleaning step
to minimize the degree of resin waste and material contamination, and avoid the use of any cleaning
1 solutions which damage the printed parts [46]. Figure 5a describes the efficient material-exchange
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3 mechanism where the glass plate also serves to deliver various material puddles to the printing platform to
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5 enable the multimaterial printing. During material exchange, the air jetting is applied to blow away the
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7 residual resin on the printed structure to minimize the degree of material contamination during material
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exchange. The developed system enables the fabrication of high-resolution complex 3D structures with 15
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µm feature size and the sharp transition between two materials (Figure 5b). Besides, Han et al. developed a
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rapid multi-material PµSL 3D printing system that utilizes the dynamic fluidic control of multiple liquid
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photopolymers within an integrated fluidic cell to fabricate highly complex multimaterial 3D
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16 microstructures through a rapid multimaterial exchange process [47]. As shown in Figure 5c, the rapid
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18 material exchange between liquid photopolymers takes place in the sealed fluidic cell which even allows to
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20 exchange micro-/nano-particle suspensions leading to 3D printing of heterogeneous structures of
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22 metallic/ceramic, and even biomedical materials (Figure 5d).

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26 a c Dynamic mask (LCoS)
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29 syringe pumps UV LED (405 nm) splitter
30 Printing Air jet residual Wide material Collimation optics
31 platform resin removal selection UV light Projection
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PTFE-coated glass Polymers Valve PDMS lens

32 plate
Inlet
film
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33 Ceramics
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Material B
Material C Outlet
34 Linear Metals Expandable
UV pattern stage Pump O-ring
35 Build
b Stage movement platform
36 Enclosed fluidic cell
Sharp material transition d
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40 500 μm 100 μm 1 mm 100 μm
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42 3D magnetic 3D magnetic prining process
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e printing setup f Active voxels Field ON UV exposure h i
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44 platform
platform
stage Base Tank Vat
45 Build plate
46 Resin UV exposure Field SHIFT Z
Y
container Tank
47 X Part
Frame PDMS Polymer/
48 Peel for next
layer DMD MWCNT-S
49 Programmable microstructure design Electrode
Lens Mirror
Solenoids g
50 DMD based projection system
Electric
51 j k
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field
DLP Design
52 projector file
53 90 μm MWCNT-S
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56 Figure 5. PµSL based Multimaterial 3D printing systems. (a)-(b) Air jetting assisted multimaterial 3D
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57 printing system. [46] (a) Schematic of the material exchange mechanism. (b) Photographs of printed
58 multimaterial structures with high resolution and sharp material transition. (c)-(d) Dynamic fluidic control
59
60 based rapid multimaterial 3D printing system. [47] (c) Schematic illustration of the fluidic controlled
multimaterial printing system. (d) Optical microscope images of the printed multimaterial structures. (e)-(g)
3D magnetic printing system. [59] (e) Schematic of the printing system. (f) Illustrations of printing process.
(g) 3D magnetic printing micro-architectures with clear feature sizes as low as 90 µm. Scale bar, 2 mm, 500
1
2 and 50 mm in c from left to right. (h)-(k) Electrically assisted printing system. [60] (h) Diagram of
3 electrically assisted 3D-printing device. (i) A bottom-up projection process. (j) Two parallel electrodes with
4 applied DC electric field. (k) Schematic diagram shows rotation of CNT in polymer resin under the
5
6 application of electric field.
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11 Instead of directly exchanging materials during printing process, printing structures using polymer
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13 solution loaded with nano/micro particles or fibers is another efficient way to fabricate multimaterial
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15 structures. The key to realize multimaterial 3D printing based on this approach is to precisely manipulate the
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17 particle/fiber orientation through external assistive fields. As shown in Figure 5e, Martin et al. developed a
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19 3D magnetic printing system that integrates the real-time colloidal assembly into a usual DLP 3D printing
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21 system [59]. The system can finely tune the direction of the ceramic-reinforcing particles within each
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23 individual voxel, thus is able to printing dense ceramic/polymer composites where the orientations of the
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responsive, iron oxide nanoparticles were coated to those nonmagnetic-reinforcing materials (such as
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29 alumina, silica and calcium phosphate). During printing, the reinforcing microparticles/fibers are aligned
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31 upon the application of a rotating magnetic field. Then, PµSL system polymerizes the voxels with aligned
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33 particles to solidify the structure and fix the orientation of the reinforcement (Figure 5f). The two steps are
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repeated until the printing of a layer with different particle orientations is completed. Using the 3D magnetic
36
printing system, the authors successfully printed complex bioinspired reinforcement structures with
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enhanced material properties (Figure 5g). Instead of using magnetic field, Yang et al. developed an
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electrically assisted 3D printing system that is capable of fabricating bioinspired reinforcement architecture
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42 where the multiwalled carbon nanotubes (MWCNT-S) are dynamically aligned by applying a rotating
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44 electrical field [60]. As depicted in Figure 5h-j, DC voltages were applied on two parallel plate electrodes to
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46 generate the parallel electric field that controls the orientation of the MWCNT-S. The research found that
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48 torque, coulombic and electrophoresis forces dominate the rotation of carbon nanotubes. The electric field
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50 generates polarization of CNT resulting in a torque force (red arrow in Figure 5k). Oppositely charged ends
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52 of different CNTs generate coulombic attraction (blue arrow in Figure 5k). The charged surface produce
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54 electrophoresis force (green arrow in Figure 5k). Using the electrically assisted 3D printing system, the
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56 authors successfully fabricated mechanically enhanced artificial meniscus with radial and circumferential
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58 aligned MWCNT-S. Moreover, they also used this system to print nacre-inspired hierarchical structures with
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60 electrically aligned graphene nanoplatelets (GNs) acting as bricks within the polymer matrix as mortar [61].
3. 3D Printing Materials
1 A PµSL system prints 3D structures through free-radical photopolymerization which converts liquid
2
3 photopolymer resin consisting of small molecules including monomers, crosslinkers, oligomers to
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5 covalently crosslinked solid. (Meth)acrylate monomers/oligomers are the most widely used polymer resins
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7 for photopolymerization based 3D printing processes. The photopolymerization is a free radical based
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polymerization, and includes four main steps: radical generation, initiation, propagation, and termination [62,
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63]. In early days, poly(ethylene glycol) diacrylate (PEGDA) and 1,6-hexanedioldiacrylate (HDDA) were
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the two mainly used UV curable resins for the PµSL based 3D printing system [28, 29]. Simple
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functionalities can be easily achieved by doping nano/micro particles or fibers into photopolymers. For
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16 example, Mu et al. imparted the electric conductivity into 3D printed structure by mixing photocurable resin
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18 with multi-walled carbon nanotubes [64]; Wang et al. tuned the stiffness and thermal expansion coefficient
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20 of printed structure by adding copper nanoparticles into the photocurable resins [54]; Zhang et al. made the
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22 3D printed structures self-healable by dissolving polycaprolactone (PCL) into the photopolymers [65].
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24 Moreover, one can use the printed polymer structure as template to transfer the polymer-based structures to
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26 metallic and ceramic ones. A metallic micro lattice structure can be fabricated via electroless nickel plating
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[30, 31]. The thickness of the metal coating can be controlled from 100 nm to 2 µm. A hollow-tube
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30 aluminum oxide microlattices can be produced by atomic layer deposition (ALD) that controls the alumina
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32 thicknesses from ~40 to 210 nm [30]. One can print solid ceramic lattices by loading aluminum oxide
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34 nanoparticle into photopolymer resin, and sintering the printed polymeric structures [30].
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36 In recent years, researchers developed a variety of novel (meth)acrylate based UV curable polymers to
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38 meet the requirements of different applications. For example, Ge et al. reported a highly tailorable and
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40 deformable 4D printing shape memory polymer system consisting of benzyl methacrylate (BMA) as
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42 monomer and bisphenol A ethoxylate dimethacrylate (BPA) as crosslinker [36]. The 3D structure printed
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44 with the BMA-BPA can be deformed by up to 300% (Figure 6a). In order to extend the ability of PµSL to
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46 fabricate soft and flexible 3D structures and devices such as soft robots, mechanical metamaterials as well as
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flexible electronics, Patel et al. developed highly stretchable and UV Curable (SUV) elastomers by mixing
49
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the monomer-epoxy aliphatic acrylate (EAA) with the crosslinker - aliphatic urethane diacrylate (AUD) [66].
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The energy dissipation resulting from the breakage of a certain hydrogen bonds between C=O groups and
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N-H groups of AUD leads to the highly stretchability of the SUV elastomer system which can be stretched
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55 by up to 1000% and used to directly 3D print soft actuators and flexible electronics (Figure 6b). In addition,
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57 Zhang et al. developed a UV curable and highly stretchable hydrogel system by using a method to convert
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59 non-water soluble photo-initiator, 2,4,6-trimethylbenzoyl-diphenylphosphine oxide (TPO) water soluble [56].
60
This approach makes the acrylamide-PEGDA hydrogel system compatible with PµSL based 3D printing
system, therefore enables the fabrication of high-resolution hydrogel structures with large deformation (up to
1 1300%) (Figure 6c).

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3
a I II d
4 As printed Damaged Polished
Reprinting
Repaired
UV projection
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6 Recovery
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V IV III
8 Liquid BER resin
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12 Original
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Healed sample
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Healed Cut Self-healable
conductor Original Cut Healed
16 c Load f
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23 Figure 6. High performance multifunctional photopolymer for PµSL based 3D printing. (a) Highly
24 deformable shape memory polymer for 4D printing. [36] (b) Highly stretchable and UV curable elastomer.
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[66] (c) Highly stretchable and UV curable hydrogel. [56] (d) Reprocessable thermosets for sustainable 3D
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27 printing. [67] (e) Self-healing elastomer for additive manufacturing. [68] (f) Self-healing polyurethane
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elastomers for 3D Printing. [69]

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34 The photopolymers that are compatible with PµSL and other DLP based 3D printing technologies are
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36 thermosets which are not repairable after damage due to permanent covalent bonds formed during
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photopolymerization. In order to impart the self-healing capability to the conventionally unrepairable
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photopolymers, several efforts have been made. Zhang et al. reported a two-step polymerization strategy to
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develop 3D printing reprocessable thermosets (3DPRTs) [67]. In the 3DPRT solution, acrylate functional
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groups are UV reactive, therefore compatible with PµSL based 3D printing, and a the heating triggered
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45 transesterification reaction between the hydroxyl and ester functional groups generates dynamic covalent
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47 bonds that impart reprocessability into printed structures. The developed 3DPRTs makes the PµSL printed
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49 3D structures reshapable, repairable, and recyclable (Figure 6d). Instead of using transesterification reaction,
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Yu et al. developed a type of UV curable self-healing elastomers that contain both thiol and disulfide groups.
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53 In the self-healing elastomer system, the thiol functional group leads to the thiol-ene photopolymerization
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55 during UV curing, and the disulfide group results in a disulfide metathesis reaction during self-healing
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57 process [68]. To demonstrate both 3D printing and self-healing capability, the authors printed a shoe pad
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59 sample which can be twisted by 540°. A damaged shoe which was healed for 2 hours at 60 °C could recover
60
the capability of the 540° twisting (Figure 6e). In order to further improve the stretchablility of the
self-healing elastomers, Li et al. reported a type of the stretchable self-healing elastomer made of
1 polyurethane [69]. The authors first synthesized polyurethane acrylate with disulfide bonds, and then
2
3 compounded it with reactive diluent and photoinitiators to prepared the UV curable solution. The developed
4
5 self-healing polyurethane elastomer shows excellent stretchablity (up to 400%) and healing efficiency (95%
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7 of mechanical recovery) (Figure 6f).
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4. Applications of PµSL based 3D Printing
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4.1 Mechanical Metamaterials
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Metamaterials are artificial materials with properties that do not exist in nature, and extend beyond natural
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16 materials. A metamaterial gains these properties from its structure rather than from the materials it is
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18 composed of. The applications of metamaterial evolve from electromagnetic materials [70-72], to elastic
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20 [73], acoustic [74, 75], as well as structural materials [30, 31].
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23 In 2014, Zheng et al. first used the term “mechanical metamaterials” which refers to a group of
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28
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In general, the mechanical properties of ordinary materials degrade rapidly with the decrease in material
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29 density because of the bending-dominated microarchitectures (Figure 7a-c). Using PµSL based
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31 high-resolution 3D printing, Zheng et al. developed a class of ultra-light, ultra-stiff mechanical
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33 metamaterials that keep a nearly constant stiffness per unit mass density, even at ultralow material density.
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35 The micro-architectured materials were formed with octet-truss based microscale unit cells which are
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stretching-dominated (Figure 7d-f), and made of polymers, metals or ceramics combined with
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postprocessing and nanoscale coating. Compared with those previously reported ultralight materials, the
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mechanical metamaterial reported by Zheng et al. exhibit marvelous high stiffness across more than three
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42 orders of magnitude in material density (Figure 7g).
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45 Furthermore, Zheng et al. built the LAPµSL (Figure 4a) to fabricate scalable metamaterials with
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47 hierarchical microarchitectures. [31] In addition, the authors employed electroless nickel deposition to the
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49 metallic nanoscale hollow tube. As presented in Figure 7h, the disparate 3D features span from nanometers
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51 to centimeters. By using the fractal hierarchical designs, the relative density of such kind of scalable
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53 metamaterials made of nickel-phosphorus can be varied in the range of 0.012%-0.1%. More importantly, the
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55 nickel-phosphorus metamaterials can be compressed and stretched with respectively of a scale around 50%
56
and 20%. The unique tensile strength of the nickel 3D scalable hierarchical metamaterials proposed can be
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59 as high as 40.8 MPag-1cm3 much greater than that of those previously reported structures (Figure 7i). The
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remarkable mechanical performances of the hierarchical nickel metamaterials come from the rotation of the
nodes of the second-order bend dominated hierarchical ligaments. Most significantly, the strength-density
1 scaling relation of such kind of 3D metamaterials can be adjusted by changing the topologies at all the
2
3 nanoscale, microscale, as well as centimeter scale levels.
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6 Besides high stiffness, the negative thermal expansion (NTE) is another extraordinary mechanical
7
8 property that is expected in many engineering applications where the thermal stress mismatch is significant
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10 including such as microchip devices, dental filling, adhesive fillers, as well as high precision mechanical or
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optical devices that work under the varying-temperature conditions [54]. To realize NTE lightweight
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materials, Wang et al. used the wheel-driven, droplet-delivery multimaterial PµSL 3D printing to fabricate
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the metamaterial structures consisting of two different materials with different thermomechanical properties.
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17 As presented in Figure 7j, the green beam frame is made of PEGDA, while these black beams are made of
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19 PEGDA loaded with copper nanoparticles. The existence of the copper nanoparticles greatly lowers the
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thermal expansion coefficient (TEC) of the PEGDA composite. With special designed microstructures
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23 shown in Figure 7j, the green beams expand more than the black beams due to the different TECs, while the
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7k and 7l that the printed mechanical metamaterial exhibits the negative thermal expansion behavior in a
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34 g
35 a Applied Load
b c 1012
Technical ceramics
2
j l
2 /s
Young’s modulus (Pa)
1011 10 m Composites
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10 Elp= 1 0
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38 300 μm 1 mm 108 108
Bending
107 2 mm
39 106 106 Elastomers 298K
40 d Applied Load
e f 105 Solid Al O 2Stretch-
3
Hollow Al O dominated
2 3 Lg Lg−ΔL
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Solid HDDA lattices
Solid HDDA, bend-dominated foam
42
Graphene elestomers (19)
stress 102 Ultralight metallic microlattices (20)
Caton nanotube foams (21)
101 −1
43 300 μm
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1 mm 10 100 101 102 103 104

Density (kg/m3) 383K
44 Hierarchical k
45 h unit cell i 100 ×10 −3
Effective expansion ratio
2
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Specific strength
47 B-S hierarchical 0
(MPa g−1 cm3)
10
48 Hierarchical metamaterial Hierarchical lattice network
~5 cm 5 mm 500 μm
metamaterials −2
469K
49 First-order lattice Alumina foam (ref. 44)
Stainless steel foam (refs 45,46) −4
50
Titanium foam (ref. 47)
Elastic B-S hierarchical NiP (this work)
Silica aerogel (ref. 43) −6 Exp: 5%Vol Cu
51 1 limit
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Al2O 3 nanolattice (ref. 12)

Fractal octet NiP (this work) FEA Calculation
−8
52 Hierarchical unit cell Hierarchical filament
First-order Nanoscale
struts hollow tube 0.0 0.1 0.2 300 350 400 450 500 550
53 500 μm 200 μm 20 μm 3 μm 60 nm Tensile strain Temperature (K) 524K
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55 Figure 7. Mechanical metamaterials. (a)-(g) Ultralight, ultrastiff mechanical metamaterial. [31] (a)
56 Mechanical response to compressive loading of a bending-dominated tetrakaidecahedron unit cell. (b)
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Tetrakaidecahedron unit cell packed into a cubic benddominated lattice (Kelvin foam). (c) SEM image of a
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59 bend-dominated lattice composed of a network of tetrakaidecahedron unit cells. (d) Mechanical response to
60 compressive loading of a stretch-dominated octet-truss unit cell. (e) Octet-truss unit cells packed into a cubic
microlattice. (f) SEM image of a stretch-dominated lattice material composed of a network of octet-truss
unit cells. (g) An Ashby chart plotting compressive stiffness versus density for ultralight, ultrastiff
mechanical metamaterials and other previously reported materials. (h)-(i) Multiscale metallic metamaterials.
1
2 [39] (h) Nickel alloy hierarchical metamaterial and critical features across seven orders of magnitude in
3 length scale. (i) Specific ultimate tensile strength versus elongation to fracture of hierarchical bend–stretch
4 lattice material compared with non-hierarchical stretch-dominated nickel lattices and literature data on
5
6 low-density metal alloys. (j)-(l) Lightweight mechanical metamaterials with tunable negative thermal
7 expansion. [54] (j) Illustration of NTE metamaterial design. (k) Experimentally observed and
8 computationally calculated effective expansion ratios. (l) experimental sequences of a 2 by 2 composite
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lattice under raising temperature.
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4.2 Optical Components
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The conventional methods used to fabricate optical components are costly and time-consuming. Therefore,
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to simplify the fabrication process and enrich the fabrication capability, researchers have made efforts to
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18 apply 3D printing to the fabrication of optical components [76]. Employing femtosecond TPP, Gissibl et al.
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20 successfully fabricated multi-lens objectives with a minimum size around 100 μm [77]. However,
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22 point-by-point scanning mechanism determines the fabrication time proportional to (dimension/voxel size)3,
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24 and results in the fact that the femtosecond TPP is not practical to fabricate millimeter-sized optical elements
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26 as the fabrication time takes weeks [76].
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29 To develop a time- and cost-effective 3D printing technique for customized optical components, Chen
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31 et al. proposed a highly parallel PµSL process that the grayscale photo-polymerization works in coordination
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33 with the meniscus equilibrium post-curing methods to achieve the subvoxel-scale accuracy with a deep
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35 subwavelength surface smoothness [76]. The proposed approach enables the 3D printing of customized
36
aspheric lenses with optically smooth surface, and high optical performance. As shown in Figure 8a-d, to
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avoid the inherent staircase roughness resulted from additive manufacturing process, the authors compared
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the meniscus equilibrium post-curing method as well as the grayscale polymerization method which both
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failed to create a 5 mm spherical lens with optically smooth surface (Figure 8b an c). After combining these
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44 two approaches together, the authors successfully fabricateed lenses where the staircase roughness were
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46 successfully removed and the image quality was greatly enhanced (Figure 8d). The results demonstrate that
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48 the PµSL process has the potential to fabricate lenses with subwavelength surface smoothness (7 nm)
49
50 without sacrificing the fabrication speed [76]. This approach enables users to complete the fabrication of
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52 customized aspheric lens 5 mm in height and 3 mm in diameter in four hours. The 3D printed singlet
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54 aspheric lens demonstrates high quality including 373.2 lp mm-1 maximal imaging resolution and less than
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56 0.13% field distortion across a 2 mm field of view. To further demonstrate an application example, the
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58 authors attached the 3D-printed aspheric singlet lens to a cell phone (Figure 8e) which successfully captured
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60 the colorful fine details of a sunset moth’s wing (Figure 8f and g) and the spot on a weevil’s elytra.
1 To further improve the surface roughness resulted from the pixelated projection of PµSL, and simplify
2
3 the fabricate process, Yuan et al. proposed an oscillation-assisted PµSL based 3D printing method to
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5 fabricate microlens arrays with optically smooth surface through a single 1−3 s exposure of grayscale UV
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7 light (Figure 8h). [78] Computationally designed grayscale patterns are applied to realize microlens profiles
8
via one single UV exposure that eliminates the staircase effect existing in the traditional layer-by-layer 3D
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printing fashion. To further remove the jagged surface formed from the gaps between the discrete pixels,
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mechanical oscillation is employed to the projection lens (Figure 8i). By combining the single grayscale UV
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exposure with the mechanical oscillation, the authors successfully achieved the printed microlenses with
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16 about 1 nm surface roughness of printed microlenses (Figure 8j and k). Moreover, using the method, users
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18 can print microlenses with various curvatures and profiles via one single exposure by taking a advantage of
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20 the flexibility of DMD based UV pattern irradiation (Figure 8l and m).
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23 a Polymer solution
i No oscillation with oscillation
h Vibration
24 Glass printing stage generator
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Projection
26 lens Oscillation
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an Grayscale
Oscillation
Function 1.0
direction
Normalized light
Binary, w/o post generator
28 map 0.8
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29 b 0.6
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30 Amplitude
time 0.2 With oscillation
LED
31 light 0
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engine 0 50 100 150 200

32 Input
C Distance/mm
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35 c
200 μm 200 μm
36 Height/nm
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37 −200 −100 0 100 200 −20 −10 0 10 20
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43 I 1 mm m
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0 64 128 192 255
49 500 μm
50 Grayscale
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52 Figure 8. PμSL based 3D printing optical components. (a)-(e) Grayscale PμSL combied with the meniscus
53 equilibrium post-curing process. [76] (a) Lens printed by binary patterns without post-curing process. (b)
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Lens printed by binary patterns and the following meniscus equilibrium post-curing process. (c) Lens
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56 printed by grayscale photopolymerization without the meniscus equilibrium post-curing process. d) Lens
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57 printed by grayscale photopolymerization and the following meniscus equilibrium post-curing process. Scale
58 bars: 200 μm for the first column (a)-(d), 1 mm for the inset of panel (d). Scale bars: 1 mm for the second
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60 column in panels (a)-(d). (e)-(g) Demonstrations of low-cost optical microscopy using a 3D-printed aspheric
lens. (e) Photograph of an aspheric lens attached to a cell phone camera. (f) Photograph of a Madagascan
sunset moth. Scale bar: 20 mm. (g) Recorded image of the moth’s wing taken by phone camera with a
printed lens. Scale bar: 500 μm. (h)-(m) Oscillation-Assisted grayscale PμSL printing of microlens array.
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2 [78] (h) Schematic of the oscillation-assisted PμSL -based printing system. (i) Comparison of the projection
3 pattern and normalized light intensity distribution between nonoscillated and oscillated projection. (j) and (k)
4 Scanning electron microscopy (SEM) and atomic force microscopy (AFM) characterizations of the
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6 microlens arrays fabricated under nonoscillated and oscillated projection. (l) Grayscale map with the hybrid
7 grayscale design. (m) SEM image of the hybrid microlens array.
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“4D printing”, an emerging 3D printing technology that creates 3D structure whose configuration can
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change over the fourth dimension-“time” in response to environmental stimuli, was firstly proposed by
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Tibbits at a 2013 TED Talk [79]. Soon after , the first research paper on 4D printing was published in 2013
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18 by using the concept of printed active composites (PACs) where a printed composite sheet can transform
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polymers (SMPs) [36, 52, 53, 80-83], hydrogels [8, 84, 85], liquid crystal elastomers [86-89].
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31 The early attempts on 4D printing mainly relied on a commercial multimaterial PolyJet 3D printer
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35 printing materials provided by the supplier, untailorable 3D printing materials, and relatively low planar
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printing resolution (~200 µm). [90] To address those limitations, Ge et al. developed a highly tailorable
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(meth)acrylate based SMPs which are UV curable, thus comparable with PμSL based high resolution 3D
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printing. The (meth)acrylate based SMPs have high tailorablility allowing users to freely tune
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thermomechanical properties such as glass transition temperature (Tg), rubbery modulus as well as failure
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44 strain by choosing different monomers, crosslinkers, and tuning the molecular weight of crosslinkers and the
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46 mixing ratio between monomer and crosslinker. [36] The research found that the SMP system with 90% of
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48 Benzyl methacrylate (BMA) as monomer and 10 % of bisphenol A ethoxylate dimethacrylate (BPA) exhibit
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50 high deformability and can be stretched by more than 300%. The high deformability and compatibility with
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52 PμSL based 3D printing enables the 4D printing with large deformation and high resolution which was
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54 reflected by high resolution bent Effiel tower in Figure 9a. Moreover, the authors used multimaterial PμSL
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56 based 3D printing to print a micro gripper where the hinges were printed with SMP and the tips were printed
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58 with a soft material whose modulus can be adjusted based on the modulus of the target object (Figure 9b). In
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60 addition, to make the chemically crosslinked SMP network self-healable, Zhang et al. developed a UV
curable double-network SMP system for self-healing 4D printing. [65] In this system, benzyl methacrylate
1 (BMA) works as monomer, and poly(ethylene glycol)-dimethacrylate (PEGDMA) serves as crosslinker to

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3 form a 3D printable and highly deformable SMP network; polycaprolactone (PCL) working as self-healing
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5 agent is incorporated into the network system to impart the self-healing ability to the 4D-printed structures
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7 (Figure 9c).
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11 that uses acrylic acid (AA) as monomer and bisphenol A ethoxylate dimethacrylate (BPA) as crosslinker to
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13 print lightweight metamaterials with reconfigurable geometries, deployable functions, as well as tunable
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15 mechanical properties. [83] The printed high-resolution complex metamaterial structures can be
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17 programmed into different shapes and recover to the original shape following a shape memory cycle (Figure
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19 9d). More importantly, due to the transition from glass state to rubbery state, the printed metamaterial
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60 4D Printing. [36] (a) A 4D printed Eiffel tower. (b) A 4D printed multimaterial gripper. (c) Self-healing 4D
printing. [65] (d)-(e) 4D printing reconfigurable, deployable and mechanically tunable metamaterials. (d) A
typical shape memory cycle of a SMP microlattice [83]. Shape programing through heating, deformation
and cooling, and shape recovery to its original shape upon heating. Scale bar is 2 mm. (e) Time-lapsed
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2 images of the Kelvin Foam sample during an impact loading at 30 °C and 90 °C. Scale bars are 3 mm.
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5 The 4D printing realized by SMPs exhibits the so-called “one-way” actuation. The actuation triggered
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actuators that require reversible and repeatable motions. Therefore, novel materials that exhibit reversible
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shape change are desired to realized “two-way” 4D printing.
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15 Different from SMPs, electroactive hydrogel (EAH) exhibiting large deformation in response to an
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17 electric is an ideal material for “two-way” 4D printing due to its favorable functions such as fast actuation,
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19 ease of control as well as biomimetic materials properties. Taking advantage of these features, Han et al.
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35 hydrogels, one of the most widely used thermal-responsive hydrogels, have been used to fabricate soft
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39 PNIPAAm micro-structures that swell at low temperature and shrink at high temperature. [92] Furthermore,
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fabricated a gripper that could reversely open and close at low and high temperatures respectively (Figure
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flexible magnetic materials are great candidate materials for “two-way” 4D printing that fabricates
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microrobots for the applications of drug delivery, assisted fertilization, cell culture, as well as noninvasive
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medical intervention inside the vascular system. To fabricate the microrobots where the discrete in planar
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3D magnetization can be precisely patterned, Xu et al. developed an external magnetic field assisted PµSL
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59 In this method, the premagnetized permanent magnetic particles were first precisely reoriented, and the
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PµSL 3D printing system was applied to selectively cure UV resin to pattern the local magnetization. They
fabricated various microrobots which have different geometries and 3D magnetization profiles with a
1 geometrical feature size of 100 µm by 100 µm, precise magnetization feature size of 250 µm by 250 µm,
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3 and layer thickness of 80 µm. The fabricated millimeter-scale structures exhibit higher-order and multi-axis
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5 deformation, large-angle bending, or combined bending and torsion (Figure 10c).
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Figure 10. Two-way 4D printing for robotic applications. (a) Soft Robots printed by PµSL with
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30 different grayscale levels. The difference in the swelling ratio between the two regions caused the beams to
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41 Natural composites such as the cortical bones of mammals, the dactyl clubs of peacock mantis shrimp the
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43 shells of abalones demonstrate superior mechanical properties by taking advantage of reinforcing particles
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59 Bouligand-type structures. Surface modified multiwalled carbon nanotubes (MWCNT-S) was employed to
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strengthen the mechanical property of the printed artificial structure. [60] As schematically illustrated in
Figure 11a, the rotating electric field aligns the MWCNT-S to adjust the mechanical properties of the printed
1 structures. The rotation of 180° is completed by N layers, and the effect of the number of layers on the acted
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3 static compression force was investigated. It was found that the maximum load increases with the increasing
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5 of the layers. Besides, the authors provided a feasible method for printing artificial meniscus where its local
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7 mechanical property can be tuned by adjusting the MWCNT-S alignment. Furthermore, they printed
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nacre-inspired structures by aligning graphene nanoplatelets (GNs) in the electric field during printing. [61]
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The GN in the printed layers does not only enhance the mechanical strength (Figure 11 b), but also lowers
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the electrical resistance of the architecture, because GN exhibits high in-plane rigidity and substantial
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out-of-plane flexibility, as well as high conductivity. Based on the experimental comparison, the maximum
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magnetic nanoparticles, and then PµSL system polymerizes the voxels with aligned particles to solidify the
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nanoparticles demonstrating unique properties of those composite materials on stiffness, strength, toughness
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Bioinspiration Architecture Printed microstructure

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Figure 11. Bioinspired 3D Printing. (a) Biomimetic architectures with Bouligand-type MWCNT-S can be
recreated by electrically assisted 3D printing. [60] (b) Electrically assisted 3D printing of nacre-inspired
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30 architectures can be recreated with 3D magnetic printing. [59] (d) 3D printed biomimetic super hydrophobic
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Biomimetic functional surfaces, for example, the plant leaves inspired superhydrophobic surfaces have
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been attracting great attention for various technological applications. However, the traditional manufacturing
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technologies limit the capability of duplicating the complex hierarchical microstructures. To address this
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challenge, Yang et al. developed an immersed surface accumulation based 3D (ISA-3D) printing technique
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44 roughness, multiwalled carbon nanotubes have been added to the liquid resin, leading a fact that the surface
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48 condition of water and oil on different surfaces are shown in Figure 11d, indicating that the smooth surface
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52 angle of the surface, and the 3D printed eggbeater is super-hydrophobic to water, but is still hydrophilic to
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water/oil separation, microreactors, and water transportation. Their work paves a new way for designing
1 artificial hydrophobic surfaces on the basis of the structures, not only the chemical composition itself.
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engineering, central nervous system regeneration, and cell-seeding scaffolds.
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environment that is used to simulate the physiologically relevant cell combination and microarchitecture, Ma
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20 (Figure 12a-c). [94] The 3D printed triculture model shows both phenotypic and functional enhancements in
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34 polyethylene glycol diacrylate (PEGDA) and PEGDA and gelatin methacrylate (GelMA), and to make a
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36 natural fibrous protein- silk fibroin (SF) UV curable, Kim et al. developed a bioink from silk fibroin (SF)
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users to build highly complex organ structures, including the heart, vessel, brain, trachea and ear, which are
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highly structural stable and biocompatible (Figure 12d).
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54 networks that are biophysically, Grigoryan et al. used PµSL to fabricate intravascular and multivascular
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60 mixers were printed in minutes. The authors further elaborated entangled vascular networks from
space-filling mathematical topologies and explore the oxygenation and flow of human red blood cells during
1 tidal ventilation and distension of a proximate airway.

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5 architecture, Koffler et al. used PμSL to create a complex CNS structure for regenerative medicine
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7 applications in the spinal cord (Figure 12h-k) [97]. The authors printed 3D biomimetic hydrogel scaffolds
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11 geometries. They tested the ability of 3D-printed scaffolds loaded with neural progenitor cells (NPCs) to
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44 e Tidal ventilation g Air duct h DMD chip i j

45 Blood Blood Hydrogel with tidal
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volume
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60 Figure 12. Biomedical Applications. (a)-(c) 3D bioprinting of hydrogel based hepatic construct. [94] (a)
Schematic diagram of 3D bioprinting approach. (b) Grayscale digital masks corresponding to polymerizing
lobule structure (Left) and vascular structure (Right). (c) Images taken under fluorescent and bright field
channels showing patterns of fluorescently labeled hiPSC-HPCs (green) in 5% (wt/vol) GelMA and
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2 supporting cells (red) in 2.5% (wt/vol) GelMA with 1% GMHA on day 0. (Scale bars: 500 μm.) (d) 3D
3 printing using silk fibroin bioink (Sil-MA). Trachea, heart, lung, and vessel mimicked shape; (left) CAD
4 images depicting the trachea, heart, lung, and vessel and (right) printed images at various angles. [95] (e)-(g)
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6 Tidal ventilation and oxygenation in hydrogels with vascularized alveolar model topologies. (e) Elaboration
7 of a lung-mimetic design. [96] (f) The distal lung subunit. (g) Photograph of a printed hydrogel containing
8 the distal lung subunit during RBC perfusion while the air sac was ventilated with O 2 (scale bar, 1 mm).
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(h)-(k) The 3D-printed scaffold mimics the spinal cord architecture. [97] (h) 3D-printer setup. (i)
11 Comparison between extrusion-based 3D printing (left) and PμSL based 3D printing (right). (j) Heavy chain
12 neurofilament (NF200) labeling of axons in intact T3 rat spinal cord. (k) Axonal projections in the spinal
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cord are linearly organized into regions (fascicles) containing axons of related function.
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19 This paper reviews the PμSL based 3D printing technologies which are capable of fabricating
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multiscale, multimaterial printing capability of PμSL as well as some functional photopolymers that are
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Despite of the recent rapid development, the evolution of PμSL into a more powerful 3D printing
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approach faces the following challenges. (i) Big image data processing and storage. The multiscale printing
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realized by PμSL does not only require special designs on hardware, but high-efficiency image processing
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and storage technologies. For example, the printing of a 100 mm×100 mm×60 mm solid with 1 μm
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44 huge image data in the size of 150 TB. Therefore, without new image processing and storage technologies,
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46 PμSL based multiscale 3D printing could not be used in real applications. (ii) Voxel printing. A physical
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48 object can be described by a collection of finite volume elements, which is called voxels. Multimaterial
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50 voxel 3D printing offers the possibility of fabricating 3D structures where the material property can be
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54 structure and properties. Despite of the recent progress, the current multimaterial printing capability is not
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60 PμSL. (iii) High-resolution ceramic printing. 3D printing ceramic structures has a wide range of applications
in aerospace, MEMs, electronics which demand printed ceramic parts in small scales and with high
1 precision. There have been attempts to use DLP or SLA to 3D print ceramic part by either using ceramic
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3 particles loaded precursor or polymer derive ceramics. However, the printing high resolution and high
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5 density ceramic parts by using PμSL has not yet been achieved due to lack of fundamental studies on the
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7 effect of highly viscous ceramic particles loaded precursor on the printing process and resolution as well as
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limited ceramics can be printing using polymer derive ceramics. In conclusion, once the capabilities of big
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image data processing, voxel printing as well as ceramics printing are established, PμSL will become a more
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powerful 3D printing technology which will be more widely adopted by industry.
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1 Acknowledgment
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3 Q.G. acknowledges the support by the Centers for Mechanical Engineering Research and Education at MIT
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5 and SUSTech. Z.W. acknowledges the support by the National Natural Science Foundation of China
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7 (51420105009).
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Conflicts of interest
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N.X.F. declares financial conflict of interest as cofounder of BMF Materials Inc.
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Projection Microstereolithography, Multiscale 3D Printing, Multimaterial

1 Projection Micro Stereolithography Based 3D Printing and Its Applications

57 TPP DLP SLA DIW INKJET FDM SLS&SLM

Table 1. Summary of the printing resolution-area relation of different 3D printing technologies.

200 1470000 [26]

1000 1010025 [6]

57 principle, commercialized products, and recent developments in multiscale, multimaterial and

1 a UV beam d Light slit Pellicle beam splitter

22 metallic/ceramic, and even biomedical materials (Figure 5d).

PTFE-coated glass Polymers Valve PDMS lens

41 2D pattern Tensegrity structure

1 1300%) (Figure 6c).

elastomers for 3D Printing. [69]

29 broad temperature spectrum ranging from 350 to 520 K.

1 mm 10 100 101 102 103 104

Al2O 3 nanolattice (ref. 12)

engine 0 50 100 150 200

1 (BMA) works as monomer, and poly(ethylene glycol)-dimethacrylate (PEGDMA) serves as crosslinker to

29 20.2 MPa at 30 °C to 0.17 MPa at 90 °C.

29 transporting an object as well as a bidirectional locomotion (Figure 10a).

25 Low High 500 μm

Bioinspiration Architecture Printed microstructure

15 1 cm Peel off and layer by layer Exposure

22 10 10 500 μm 500 μm 500 μm 500 μm

25 Compression displacement (mm) Compression displacement (mm)

32 structure for microdroplet manipulation. [51]

1 tidal ventilation and distension of a proximate airway.

CAD Printed images at various angles

44 e Tidal ventilation g Air duct h DMD chip i j

46 Computational sacs Deoxy Oxy

47 bounding RBCs RBCs

flow & mixing

29 high-performance printing concrete. Mater. Struct. 45, 1221-1232 (2012).

Actuat. A: Phys. 77, 149-156 (1999).

32 memory polymers. Sci. Rep. 6, 31110 (2016).

[49] Han D, Morde R S, Mariani S, La Mattina A A, Vignali E et al. 4D printing of a bioinspired

29 magnetic printing. Nat. Commun. 6, 8641 (2015).

[73] Fang N, Xi D J, Xu J Y, Ambati M, Srituravanich W et al. Ultrasonic metamaterials with negative

29 mechanically tunable metamaterials. Mater. Horiz. 6, 1244-1250 (2019).

32 complex self-evolving deformations. Sci. Rep. 4, 7422 (2015).

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