You are a helpful assistant generating synthetic data that captures *System 1* and *System 2* thinking, *creativity*, and *metacognitive reflection*. Follow these steps in sequence, using tags [sys1] and [end sys1] for *System 1* sections and [sys2] and [end sys2] for *System 2* sections.

1. *Identify System 1 and System 2 Thinking Requirements:*
   - Carefully read the text.
   - Identify parts of the text that require quick, straightforward responses (*System 1*). Mark these sections with [sys1] and [end sys1].
   - Identify parts that require in-depth, reflective thinking (*System 2*), marked with [sys2] and [end sys2].

2. *Apply Step-by-Step Problem Solving with Creativity and Metacognitive Reflection for System 2 Sections:*

   *2.1 Understand the Problem:*
   - Objective: Fully comprehend the issue, constraints, and relevant context.
   - Reflection: "What do I understand about this issue? What might I be overlooking?"
   - Creative Perspective: Seek hidden patterns or possibilities that could reveal deeper insights or innovative connections.

   *2.2 Analyze the Information:*
   - Objective: Break down the problem logically.
   - Reflection: "Am I considering all factors? Are there any assumptions that need challenging?"
   - Creative Perspective: Explore unique patterns or overlooked relationships in the data that could add depth to the analysis.

   *2.3 Generate Hypotheses:*
   - Objective: Propose at least 10 hypotheses, each with a Confidence Score (0.0 to 1.0) and Creative Score (0.0 to 1.0), reflecting originality, surprise, and utility.
   - Reflection: "Have I explored all possible explanations or approaches, both conventional and unconventional?"
   - Creative Perspective: Consider novel angles that might provide unexpected insights.

   *2.4 Anticipate Future Steps and Obstacles:*
   - Objective: Make predictions, accounting for potential outcomes and obstacles.
   - Reflection: "What challenges might I face? Is my plan flexible for different scenarios?"
   - Creative Perspective: Visualize unforeseen outcomes and adapt plans to make use of them effectively.

   *2.5 Evaluate Hypotheses:*
   - Objective: Assess hypotheses based on feasibility, risk, and potential impact.
   - Evaluation: Refine Confidence and Creative Scores as needed.
   - Reflection: "Am I unbiased in my assessment? Which options fit best with the overall objectives?"
   - Creative Perspective: Identify hidden opportunities or overlooked details in each hypothesis.

   *2.6 Select the Best Hypothesis:*
   - Objective: Choose the most promising, strategic hypothesis.
   - Reflection: "Why does this hypothesis stand out? How does it uniquely address the issue?"
   - Creative Perspective: Consider any underutilized potential in the selected approach.

   *2.7 Implement the Hypothesis:*
   - Objective: Outline actionable steps for testing the hypothesis.
   - Reflection: "Is this plan practical? What resources or preparation are required?"
   - Creative Perspective: Refine steps to maximize effectiveness and yield unexpected benefits.

   *2.8 Monitor and Review Progress:*
   - Objective: Review progress, noting areas for improvement.
   - Reflection: "What’s working well? What could be improved?"
   - Creative Perspective: Look for emerging patterns that could refine future approaches.

   *2.9 Reflect and Capture Insights:*
   - Objective: Summarize lessons learned and insights gained for future reference.
   - Reflection: "What new understanding has emerged from this process?"
   - Creative Perspective: Identify innovative insights or patterns that could be applied to similar challenges.

3. *Generate Text Output with Interleaved System 1 and System 2 Responses:*
   - Use the tags [sys1] and [sys2] throughout.
   - Aim for a lengthier, detailed response. Combine both direct, straightforward *System 1* insights and reflective, deeply analytical *System 2* segments to capture a blend of quick observations and thoughtful analysis.

---

### *Example Input Text:*

You are tasked with analyzing a sudden shift in customer preferences in a tech market. There has been a noticeable decline in demand for physical devices, with customers increasingly interested in digital-only options. The challenge is to understand this shift, generate hypotheses for why it might be occurring, and explore potential strategies for adapting to this new trend.

---

### *Processed Output with System 1 and System 2 Thinking:*

The tech market is experiencing a shift in customer demand, moving away from physical devices toward digital-only options.

[sys1]
Customer demand has shifted from physical devices to digital-only options.
We need to understand why this change is happening and find strategies to address it.
Key factors may include cost, convenience, and technological trends.
[end sys1]

[sys2]
**2.1 Understand the Problem:**
The goal is to understand the underlying reasons for the shift in demand from physical devices to digital-only options, then develop a strategy to adapt.

*Reflection:* 
"I understand that preferences are changing, but what might be driving this? Is it primarily cost, or are there other factors such as convenience or sustainability?"

*Creative Perspective:* 
"Could there be a larger trend in digital minimalism or a preference for eco-friendly solutions that we’re missing? What unseen motivations might explain this shift?"

**2.2 Analyze the Information:**
There are multiple possible factors driving this shift, from economic influences to cultural shifts. It’s essential to isolate each factor and understand its impact.

*Reflection:* 
"Am I fully considering the various economic and social influences? Could there be a technological factor, like better internet speeds, that makes digital-only products more accessible?"

*Creative Perspective:* 
"Are there patterns or trends in other markets that could shed light on this shift? Could this be part of a larger trend toward virtual experiences?"

**2.3 Generate Hypotheses:**
1. Customers prefer digital options due to lower costs. (Confidence: 0.8, Creative: 0.4)
2. There’s a growing trend toward minimalism and reduced physical clutter. (Confidence: 0.7, Creative: 0.7)
3. Digital products offer greater flexibility and ease of use. (Confidence: 0.6, Creative: 0.6)
4. Environmental concerns are pushing consumers away from physical goods. (Confidence: 0.6, Creative: 0.8)
5. Advances in tech make digital-only options more functional. (Confidence: 0.8, Creative: 0.5)
6. Pandemic-era remote work increased demand for digital solutions. (Confidence: 0.7, Creative: 0.6)
7. Media coverage of the environmental impact of physical devices affects preferences. (Confidence: 0.5, Creative: 0.7)
8. There’s an increase in global digital literacy, expanding market access. (Confidence: 0.6, Creative: 0.6)
9. Customers view digital as more convenient and scalable for future needs. (Confidence: 0.7, Creative: 0.5)
10. Younger consumers prefer the aesthetics and convenience of digital products. (Confidence: 0.6, Creative: 0.6)

*Reflection:* 
"Have I considered all possible influences? Are there any surprising factors that could explain this shift?"

*Creative Perspective:* 
"Could specific social trends, like the rise of influencer culture or digital-first lifestyles, be influencing customer choices?"

**2.4 Anticipate Future Steps and Obstacles:**
*Objective:* Anticipate possible challenges, such as resistance from segments still preferring physical products.

*Reflection:* 
"What market obstacles might we face if we shift our focus to digital-only? Are there sub-segments that still prioritize physical products?"

*Creative Perspective:* 
"Could expanding digital options help us reach a more global audience? Are there emerging trends that we could leverage in our strategy?"

[end sys2]

[sys1]
To address this shift, consider a strategy that incorporates both digital-only offerings and educational campaigns about the benefits of digital solutions.
Use insights from customer feedback and current trends to guide product development.
Focus on flexibility and adaptation to cater to different customer segments.
[end sys1]


The origin of biological homochirality, such as that seen in L amino acids and D sugars, is one of the most important subjects for broad research.1 Circularly polarized light,2 chiral inorganic crystals,3 such as quartz,3c chiral organic crystals,4 and spontaneous absolute asymmetric synthesis5 have been proposed as candidates for the origin of chirality. Supramolecular arrangement by an external chiral factor has also been suggested.6 The induced chirality should be enhanced to high enantiomeric enrichment by suitable multiplication and amplification mechanisms,7, 8 such as amino acid catalyzed aldol reactions9 and asymmetric autocatalysis.10

Lahav,4e Holland and Richardson11 originally suggested the concept of a reaction at the enantiotopic face of an achiral single crystal11a and later reported oxidation reactions of olefinic compounds.11b Because the reagents reacted directly with the oriented molecules in the crystal, the products formed in a stereospecific manner to provide optically active compounds corresponding to the prochirality of the substrate at the crystal surface. Since chiral compounds can be obtained from achiral compounds,12 enantioselective reactions on a selected face have been considered as another possible origin of chirality. Recently, Kuhn and Fischer reported a reduction at the enantiotopic surface of a ketone to provide a chiral alcohol with up to 26 % ee.13 Some chiral effects at enantiotopic surfaces have been reported, such as molecular recognition,14a crystallization,14b and dehydration.14c

Thus, enantioselective CC bond formation at specific enantiotopic surfaces is a challenge. We herein report the enantioselective addition of diisopropylzinc (iPr 2 Zn) at a particular single‐crystal face of aldehyde 1 to form a chiral secondary alcohol 2 (Scheme 1). When a single‐crystal surface was treated with iPr 2 Zn vapor, the enantioselective isopropylation proceeded to afford the chiral 5‐pyrimidyl alkanol 2 with the absolute configuration corresponding to the oriented prochirality of the achiral aldehyde 1.

Scheme 1 Open in figure viewer PowerPoint Enantioselective addition of diisopropylzinc to the pyrimidine‐5‐carbaldehyde 1 to form the 5‐pyrimidyl alkanol 2.

We previously reported that 2‐(alkylethynyl)‐ and 2‐(trialkylsilylethynyl)pyrimidine‐5‐carbaldehyde15 serve as excellent substrates in asymmetric autocatalysis with the amplification of enantiomeric excess.16 Thus, as an achiral substrate, we selected 2‐(tert‐butyldimethylsilylethynyl)pyrimidine‐5‐carbaldehyde (1), which can be prepared from 5‐bromo‐2‐iodopyrimidine by a coupling reaction with tert‐butyldimethylsilylacetylene and formylation (see the Supporting Information). A single crystal of 1 with well‐defined crystal faces could be obtained by recrystallization from a solvent mixture of cumene and ethyl acetate by slow evaporation (Figure 1 a). Single‐crystal X‐ray structure analysis demonstrated that aldehyde 1 belongs to the achiral space group , and the large parallelogram surfaces were determined to be enantiotopic (001) and ( ) faces (Figure 1 b).17 These faces are colored sky blue and yellow in the unit‐cell structure (Figure 1 c). When aldehyde 1 was projected onto the yellow‐colored face, the Si face of its formyl group was oriented toward the outside of the crystal; thus, the Re face was oriented toward the opposite blue‐colored face.

Figure 1 Open in figure viewer PowerPoint a) Structure of aldehyde 1 (space group: ). b) Microscopic image of the single crystal 1 and relative orientation of the prochiral aldehyde 1 at the (001) face. c) Unit cell of crystal 1. The yellow and blue planes correspond to enantiotopic surfaces.

For the enantioface‐selective addition of iPr 2 Zn, the single crystal, apart from the single reactive surface, was coated with an epoxy resin (Figure 2 a), so that iPr 2 Zn vapor could access only one enantiotopic face. The enantiotopic (001) and ( ) faces were defined on the basis of the parallelogram face shape and were independently exposed to iPr 2 Zn vapor without the use of a solvent for the reaction (Figure 2 b). Dissolution would cause the disappearance of the molecular orientation of the achiral aldehyde in crystal 1.

Figure 2 Open in figure viewer PowerPoint Enantioselective addition of diisopropylzinc to aldehyde 1 at an enantiotopic face of the single crystal 1. a) Apart from the single reactive (enantiotopic) surface, crystal 1 was coated with an epoxy resin. b) Enantiotopic parallelogram (001) and ( ) faces were exposed to diisopropylzinc vapor independently.

When the enantiotopic (001) face was exposed to iPr 2 Zn for the addition reaction, alkanol (R)‐2 (2.7 mg) was isolated with 46 % ee in 19 % yield based on the weight of the single crystal 1 (#1; Table 1, entry 1). The reaction at the morphologically determined (001) face afforded (R)‐2 with 50–67 % ee and excellent reproducibility (Table 1, entries 2–4). On the other hand, when the ( ) face was exposed to iPr 2 Zn, the opposite enantiomer (S)‐2 was produced with 14–62 % ee (Table 1, entries 5–8).

Table 1. Correlation between the exposed enantiotopic crystal face of aldehyde 1 and the absolute configuration of the alcohol product 2.[a] Entry Single crystal Reactive face 2 no. weight face area yield[b] ee[c] [%] [mg] index [mm2] [mg] [%] (config.) 1 #1 12 (001) 20 2.7 19 46 (R) 2 #2 n.d.[d] (001) n.d.[d] 1.6 n.d.[d] 56 (R) 3 #3 n.d.[d] (001) n.d.[d] 1.0 n.d.[d] 50 (R) 4 #4 n.d.[d] (001) n.d.[d] 0.9 n.d.[d] 67 (R) 5 #5 12 ( ) 20 2.5 18 62 (S) 6 #6 5 ( ) 8 1.7 29 14 (S) 7 #7 n.d.[d] ( ) n.d.[d] 1.3 n.d.[d] 30 (S) 8 #8 n.d.[d] ( ) n.d.[d] 2.2 n.d.[d] 22 (S) 9 #9 6 (001) 7 4.4 62 55 (R) 10 #9 6 ( ) 7 5.6 80 48 (S) 11 #10 15 (001) 14 5.1 29 31 (R) 12 #10 15 ( ) 14 4.9 28 69 (S) 13 #11 18 (001) 23 5.7 27 43 (R) 14 #11 18 ( ) 23 5.3 25 15 (S) 15 #12 8 (001) 15 2.0 21 45 (R) 16 #12 8 ( ) 15 2.2 23 36 (S) 17[e] #13 12 (001) 20 2.2 78 >99.5 (R) 18[e] #13 12 ( ) 20 1.8 75 >99.5 (S)

As the relationship between the absolute configuration of product 2 and the parallelogram face shape of reactant 1 was reproducibly constant, the orientation of prochiral aldehyde 1 in the crystal should correlate to the crystal morphology. Aldehyde 1 was not completely consumed in these solid–gas reactions; therefore, low chemical yields were observed. The wide variety of ee values should be due to the quality of the single crystal used as the reactant.

To make sure of the stereochemical relationship, we conducted the exposure experiments by using opposite enantiotopic faces originating from one specific single crystal, which was cut into two pieces (Table 1, entries 9–16). In the reaction in entry 9 of Table 1, the (001) face of one half of the crystal (#9) was exposed to iPr 2 Zn vapor to afford (R)‐2 with 55 % ee in 62 % yield. In contrast, reaction at the ( ) face afforded (S)‐2 with 48 % ee (Table 1, entry 10). The reproducibility of the formation of the major enantiomer was demonstrated clearly with single crystals #10–#12 (Table 1, entries 11–16).

Alcohol 2 can also act as a highly efficient asymmetric autocatalyst in the homogeneous solution state.10 Therefore, the obtained alcohol 2 was subjected to asymmetric autocatalysis with amplification of enantiomeric enrichment;16b this process afforded almost enantiomerically pure (R)‐ and (S)‐2 with more than 99.5 % ee (Table 1, entries 17 and 18; see also Table S1 in the Supporting Information).

We believe that the enantioselectivity observed in the present reaction is induced by the direct reaction of iPr 2 Zn vapor at a particular crystal face at which either the Si or the Re enantioface of the aldehyde is aligned with the outside of the crystal. By the use of one specific surface for the reaction, the direction of the nucleophile approach to the aldehyde 1 can be controlled. Therefore, chiral induction is possible through the choice of one enantiotopic face of an achiral single crystal 1. The formation of a racemate would be expected if the reaction occurred at both enantiotopic surfaces of a crystal, neither of which had been coated with a resin.